Simon became the CFL's all-time leading receiver as he caught five passes for 105 yards, helping the Lions to a 33-16 victory over the Winnipeg Blue Bombers.
The defending-champion Lions faced little difficulty as they led the 2011 Grey Cup rematch from start to finish.
"This is the ultimate goal — to win," said Simon. "If we'd gotten the record and we didn't win, that would have left a sour taste in my mouth."
The star slotback set the record on a 56-yard pass from Travis Lulay 4:57 into the fourth quarter.
The 36-year-old Simon was all alone as he hauled in the Lulay bomb along the sidelines and brought the ball to the Winnipeg 23-yard line.
Simon bettered the record of 15,153 yards held by retired Bomber great Milt Stegall, who was on hand for the game. The Lion now has 15,192 yards in his career.
"I'm proud of the way I played (and) the legacy I'm going to leave," said Simon. "I'm proud of being from Johnstown, Pa., a place that nobody's heard of."
Although Simon did not get into the end zone himself, his first and final receptions on the night helped set up 10 points. After he made his first catch for just five yards in the first quarter, Travis Lulay opened the scoring on a five-yard touchdown run.
Then, after Simon entered the history books, Paul McCallum kicked a field goal to put the Lions ahead 26-10.
The record-setting catch came after Simon made three unsuccessful attempts. He could not control two passes and Winnipeg's Jonathan Hefney interfered with him on another, drawing a penalty.
"They're a good defence, but I knew that I'd get opportunities to make plays," said Simon. "They gave me a couple and I didn't capitalize on them, but I finally got (the ball) and made it work."
Seconds after the historic catch, Simon was hugged by his 18-year-old son Gervon, who travelled from Johnstown to witness history.
Stegall, now a TV broadcaster, was on hand for the game and participated in a brief on-field ceremony that included CFL commissioner Mark Cohon and Lions general manager Wally Buono.
"It's an amazing feeling," said Simon of the record. "I'm excited for the organization to do it at home. I'm excited for the fans that they were here to share in this moment with me."
Simon stole the show from Lulay, who ran for two touchdowns and threw for another. But Lulay did not seem to mind. He was glad to be part of history.
"I thought it might drift out of bounds," said Lulay of the record-setting toss. "He made the play, kept his feet in bounds and got the yards he needed. It's awesome to be on the throwing end of that kind of record."
Lulay, chosen the CFL's most outstanding player in 2011, picked up where he left off at the end of last season as he completed 17 of 25 passes for 233 yards and gained another 44 on the ground.
Simon and Lulay helped the Lions get off to the hot start they were seeking after going 0-5 out of the gate last year.
McCallum accounted for the rest of the Lions' scoring as he kicked four field goals and two converts.
Winnipeg backup quarterback Alex Brink threw a pair of touchdowns. The first to Terrence Edwards in the third quarter and the second to Chris Matthews in the final minute.
"We didn't score enough points," said Winnipeg coach Paul LaPolice. "It's not just Alex (Brink), it's everybody offensively. We've got to play better in all three phases."
A Justin Palardy field goal was the only other offence that the injury-riddled Bombers could muster.
Shortly before half-time, Winnipeg lost starting QB Buck Pierce as he left the game holding his right knee. Pierce departed one play after being sacked by Keron Williams for the second time. Altogether, the Lions recorded four sacks in the first half.
"He hurt his lower leg," said LaPolice. "It swelled up. We're going to keep an eye on him. I think it was that one hit he took in the second quarter."
The oft-injured Pierce, who was released by the Lions following the 2010 season because of his health struggles, managed only three completions on nine attempts for 11 yards.
Lulay secured the victory early in the fourth quarter, after Tim Brown romped 59 yards on a punt return and the Lions gained 15 more on the play as Dustin Doe was penalized for a horse-collar tackle. Three plays later, Lulay ran into the end zone from seven yards out to stake the Lions to a 23-10 advantage.
"It wasn't a perfect night offensively but we put enough points on the board," said Lulay.
The Lions helped new coach Mike Benevides post a win in his regular-season debut. Benevides replaced Buono last December after the legendary coach stepped down after 22 seasons with Calgary and B.C. and six Grey Cups.
"It felt great," Benevides said of his inaugural triumph. "I was really proud of all the guys fighting through the adversity."
Benevides was disappointed that the game stopped after Simon's record-setting catch, because he thought the ceremony thwarted his club's momentum. But the rookie coach, who ran on to the field to congratulate the 14-year veteran, did not mind.
"At the end of the night it was Geroy Simon Night," Benevides said. "It was a treat to watch him get the record and I'm proud of the team for being in his corner all night."
Notes: Before the game, the Lions raised their 2011 Grey Cup champions banner. ... The B.C. Place roof was closed. ... The Lions recorded four sacks while the Bombers had three. Both Lulay and Brink threw an interception.