Devin Hester scored on an 82-yard punt return with two minutes and 58 seconds remaining to complete the Bears' amazing fightback, which also included a pair of fumble return touchdowns by an opportunisitic defense.
"We just kept playing hard," Bears linebacker Brian Urlacher said.
"We never gave up and we made some plays when we had to."
The Bears improved to a National Football League leading 6-0, their best start in 20 years despite trailing 23-3 in the dying seconds of the third quarter.
"It's pretty exciting. We thought we would win when we came out here but not like this," Urlacher said.
The Bears had lost the past 16 games in which they trailed in the fourth quarter but snapped that NFL-longest active streak despite an attack that had the ball barely 20 minutes and moved only 168 yards.
Arizona's collapse also set a record.
There squandering of a 14-0 first quarter lead for the second week in a row, brought the Cardinals to 1-5, winless after taking their opener.
No other team in NFL history had thrown away two such leads in a season.
"Somehow we always keep hurting ourselves," Arizona quarterback Matt Leinart said.
"There's no one to blame for the loss. It's a team effort. It's frustrating to have these games won and then they come back and we lose it.
More soul searching for Matt
"It's frustrating. It really is."
Cardinals coach Dennis Green screamed during his news conference, a meltdown under the weight of frustration, anger and failure.
"The Bears are what we thought they were," Green said. "If you want to crown them, crown their ass. They are who we thought they were.
"And we let them off the hook."
The Bears trailed by 20-0 at half-time and by the same margin until defender Mike Brown returned a Leinart fumble three yards for a touchdown on the last play from scrimmage in the third quarter, lifting Chicago within 23-10.
"I didn't feel like I was even getting blocked. I was able to make a lot of one-on-one tackles," Urlacher said. "We're a good defense. We had to make plays when we had to."
Chicago's defense struck again with five minutes remaining in the fourth quarter.
Urlacher pulled the ball loose from Cardinals' running back Edgerrin James forcing the rusher's first fumble in a year, and Charles Tillman ran the ball back 40 yards for a touchdown to cut the deficit to 23-17.
"They showed again why they are an awesome defense. They made plays when they needed to," Leinart said. "We just have to find what we're good at and stick with it. It's tough when you are 1-5. It hurts inside."
The Bears' defense held firm again and forced an Arizona punt which Hester grabbed and raced back for a touchdown, eluding defenders thanks to key blocks and impressive moves to give the Bears a 24-23 lead.
The Cardinals had a chance to snatch victory in the final moments, but Arizona kicker Neil Rackers missed a 40-yard field goal wide left of the uprights with 48 seconds remaining, snuffing out the Cardinals' last hope to give the Bears their miracle victory.
"Everything was going our way," Urlacher said. "I thought we would get up in his face and pressure him."
Thomas Jones on the attack
It was the first time in Bears' history the club had erased a 20-point deficit in the second half to win.
Chicago's defenders kept Arizona rusher James to 56 yards on 36 rushes, the fewest yards gained in a game by a rusher with so many carries in NFL history.
"It's a gut check time," Leinart said. "We have to make a choice. We have to keep fighting back. We know how good we can be. We played awesome against the number one team. We showed what we are capable of. We just have to go do it.
"We have to learn from this. We have to learn how to finish off teams."
Leinart connected with Bryant Johnson on an 11-yard touchdown pass 7:54 into the game to give the Cardinals a 7-0 lead and hit Anquan Boldin on a 26-yard touchdown throw 6:12 later to boost the Arizona edge to 14-0.
The former University of Southern California star connected on 8-of-9 passes for 46 yards in the first quarter and for the game was 24-of-42 for 232 yards.