Striker wrestled Kurt Angle, using the name Matt Martel, in an invitational match on the February 24, 2005 episode of WWE SmackDown! in Philadelphia, Pennsylvania. Striker made a WWE second appearance on the July 11, 2005 episode of Raw to face Angle for a second time, again using the name Matt Martel. His news coverage was played up by Angle, who told the audience that Martel was really Matt Striker, and Angle defeated him again in under three minutes. The following week, he appeared on Raw again, still claiming to be called Matt Martel, and challenged Angle again. Angle exposed him as Matt Striker again, before defeating him for the third consecutive time. Striker went on to compete on Heat.
Striker developed a heel (villainous) teacher gimmick, calling WWE his school and hosting a segment called Matt Striker's Classroom on Raw, which debuted on December 12. During the segment he ridiculed the audience, and treated the crowd as intellectual inferiors. During a match against Lance Cade at an untelevised event on December 18, Striker suffered a shoulder injury. He was out of action until January 23, 2006, when he continued his Classroom segments once again, and then appeared mainly on Heat for several weeks.
Striker would reappear on Raw on April 17 for another classroom segment where he claimed that "school is cool". Carlito, another wrestler, took exception to Striker's statement, and spat an apple in Striker's face, in keeping with Carlito's gimmick. Striker returned to Raw in-ring action on April 24 and participated in a six-man tag team match, in which he, Chris Masters and Shelton Benjamin were defeated by Carlito, Rob Van Dam, and Charlie Haas. During the Backlash pay-per-view, Striker hosted an edition of his classroom segment, with Eugene, who in storyline was mentally impaired, as his guest. Eugene attacked Striker during the segment, which led to Striker attacking Eugene with a dictionary the following night on Raw. The scripted feud between the two also involved Carlito, who attacked both Eugene and Striker after Eugene inadvertently caused Carlito to lose a match to Striker by Disqualification on the May 8 episode of Raw. The feud between the two ended when Eugene gained a mentor in "Hacksaw" Jim Duggan and defeated Striker, after losing to him only two weeks before. Following his loss to Eugene, Striker attacked him, but was stopped by Duggan, and ran away.
Striker appeared only rarely on Raw throughout June and July, and his final match for the brand was on July 31, when he was quickly defeated by John Cena.
At the end of August 2006, Striker left the Raw brand to join ECW, making his debut on August 23. He continued his Classroom segment on ECW, which provoked a feud with The Sandman as Striker insulted him. Striker made his in-ring debut for the brand on the September 19, 2006 episode of ECW, teaming up with Mike Knox and Test to face Tommy Dreamer, Sabu, and The Sandman. Striker, Knox, and Test lost the match by disqualification due to Test pushing the referee. Striker continued his feud with The Sandman until the October 17 episode of ECW, when The Sandman defeated Striker in a Singapore Cane on a Pole match. At the December to Dismember pay-per-view, Striker faced Balls Mahoney in a "Striker's Rules" match, which meant that no eye gouging, hair pulling, top rope attacks, or foul language was allowed. Despite the match being of his own creation, Striker was pinned by Mahoney. Striker and Mahoney continued their rivalry until December 19, when Striker defeated Mahoney on ECW.
On February 6, Striker aligned himself with Mr. McMahon's New Breed stable (faction), along with Elijah Burke, Kevin Thorn, and Marcus Cor Von. The New Breed immediately engaged themselves in a feud with the ECW Originals (Rob Van Dam, Tommy Dreamer, Sabu and The Sandman). Different members of the New Breeds wrestled members of the ECW originals over several weeks, leading up to WrestleMania 23. At WrestleMania, the New Breed was defeated by the ECW Originals in an 8-man tag team match, but won a rematch on the following episode of ECW. In the midst of the feud with the ECW Originals, tension began to appear between the leader Elijah Burke and Striker, after Striker and Cor Von were defeated by the debuting Major Brothers. As a result, Striker began trying to avenge the loss to the Major Brothers, and defeated Brett Major on the May 22 episode of ECW. The feud with the Originals lost momentum, however, as Sabu was released from his WWE contract in mid-May, and at the One Night Stand pay-per-view, the feud ended when Striker, Cor Von, and Burke lost to Dreamer, Sandman, and CM Punk in a tables match.
On June 12, Striker was defeated by The Boogeyman in a singles match, and two weeks later, The Boogeyman attacked him during an edition of Piper's Pit, both times dropping worms from his mouth into Striker's. On July 10, Striker invited Boogeyman to the ring to educate him on worms, only to bring out the debuting Big Daddy V to attack Boogeyman. Striker then formed an alliance with Big Daddy V that lasted until March 2008, and acted as Big Daddy V's manager, regularly accompanying him to the ring. In November, Striker and Big Daddy V started a feud with Kane, after Kane attacked Striker. The feud saw Striker and Big Daddy V take on Kane in a handicap match, and also saw the pair align briefly with Mark Henry. Henry helped Big Daddy V win a match against Kane on the November 27 episode of ECW, and in return, Striker refereed a match between Henry and The Undertaker, and refused to count a pinfall against Henry.
As part of the 2008 WWE Supplemental Draft in June 2008, Striker was drafted back to the Raw brand. Once the SmackDown color commentator, Mick Foley, was storyline injured by Edge, however, Tazz moved to SmackDown to fill in for Foley, who had actually left the WWE in real life, and Striker returned to ECW to take over Tazz's duties as color commentator, thus turning Striker face and ending his in ring career at the same time. He made his commentary debut on the August 5 episode of ECW. Striker and his commentary partner, Todd Grisham, won the 2008 Slammy Award for the Announce Team of the Year. On the April 7, 2009 episode of ECW, Grisham and Striker's commentary partnership came to an end when Josh Mathews debuted as the new play-by-play commentator, to replace Grisham who was moved to the SmackDown brand. In addition to commentating on ECW on SyFy and ECW pay-per-view matches, Striker and Mathews represented the ECW brand on WWE Superstars every week, which started with the inaugural episode on April 16, 2009.
On October 27, 2009 it was announced that Striker would move from commentary on ECW to SmackDown, reuniting with Grisham. The move was made to help accommodate Jim Ross, who had been taking time off to deal with his recent Bell's palsy attack. In November, Striker replaced Jerry Lawler on commentary for Raw for one night, after Lawler was attacked by Sheamus, and in storyline, was unable to continue.
On June 7, 2010, Striker appeared on Raw for the "viewers choice" episode, announcing the results of the votes. At the end of the show, Striker was attacked by the season one NXT rookies, along with the commentators and Justin Roberts, the ring announcer. In October, Striker and Grisham were joined by Michael Cole on SmackDown, forming a three-man announce team. Striker remained a SmackDown commentator until he was replaced in early February 2011 by Booker T.
On the inaugural episode of NXT on February 23, 2010, Striker was announced as the host of the show and he conducted an interview with wrestler Daniel Bryan. As well as interviewing the wrestlers, Striker's host role resulted in him acting as the Master of Ceremonies for the Pro's Poll and for the various challenges each week, explaining the rules and announcing the winners.
In March 2011, Striker gained a co-host for the fifth season of NXT in the form of Maryse. On the June 2 episode of Superstars, Striker appeared as the new agent of Tyson Kidd and managed Kidd for that single episode of Superstars.
Striker wrestled his first match in three years on the August 2, 2011 episode of NXT, teaming with Titus O'Neil in a winning effort against Derrick Bateman and Darren Young in a tag team match, turning face for the first time since his debut. He fought Young in the next two weeks, but Young emerged victorious both times. Striker later teamed up with William Regal to face Young and JTG, but Striker and Regal were unsuccessful in winning the match.
Striker was reunited with his former broadcast partner Josh Mathews on the November 10, 2011 episode of WWE Superstars, commentating on both the Raw and SmackDown portions of the show.
Meanwhile, as NXT host, Striker was frequently bullied and even assaulted by troublemakers Curt Hawkins and Tyler Reks, eventually forcing him to hand over match booking responsibilities to William Regal on the February 29 episode of NXT Redemption even though Striker would remain as NXT host. On the March 21 episode of NXT Redemption, after Maxine and Johnny Curtis knocked out Striker with chloroform, Striker was kidnapped (kayfabe) by unknown persons, later revealed to be Hawkins and Reks, who intended to blackmail Maxine into using her charms to get Regal to leave them alone. Despite apparently being kidnapped, Striker continued to commentate on Superstars, with the explanation given being that to keep his kidnapping a secret, WWE hired a body double to assume Striker's duties. Striker was rescued by Derrick Bateman and Kaitlyn on the April 11 episode of NXT.
After hosting NXT, Striker began interviewing WWE employees on Raw and SmackDown. During the summer of 2012, Striker became the host of WWE After Burn for international broadcasts. On the October 12 episode of SmackDown, Stirker tried to interview Team Hell No, after Kane fought Dolph Ziggler in a match, but was placed in the No! Lock by Daniel Bryan and chokeslammed by Kane. On the October 15 episode of Raw, Striker was placed in a match against Kane by Raw General Manager AJ Lee, in which he was defeated. On the January 28th episode of Raw he was knocked out by Big Show while attempting an in ring interview. On June 20, Matt Striker revealed on his twitter that his WWE contract will not be renewed.