With a 13-yard touchdown catch in the fourth quarter of Dallas' 38-14 win Thursday over the Washington Redskins, Bryant surpassed Bob Hayes, who had 71 touchdown catches in his Hall of Fame career with the Cowboys.
On the first play of the fourth quarter, Bryant faked inside before cutting back out and leaped high for a fade from Dak Prescott over Washington cornerback Bashaud Breeland to give the Cowboys a 24-7 lead.
Bryant's 61-yard effort for the night included a 24-yard catch that set up the record-setting TD.
"I was talking about that demeanor and that attitude that we carried,'' Prescott said. "I give him credit. He kind of brought it this week and pretty much tonight and you kind of felt it early.''
After tying Hayes' mark in the Oct. 22 win against the San Francisco 49ers, Bryant went five games without a touchdown reception before Thursday, which was the longest dry spell of his career. He went four games without a touchdown catch in 2010, his rookie year, and 2012.
"It is special," Prescott said. "He deserves it. He is a guy that works hard, is very passionate with everything that he does. I am happy for him."
He entered Thursday's game with 53 catches for 578 yards and four touchdowns in 11 games. In 13 games against Washington prior to tonight's game, he had 62 catches for 916 yards and seven touchdowns.
"Dez was outstanding," owner and general manager Jerry Jones said. "When he fell to us, we certainly felt it was an opportunity for us in the draft. That's not the same Dez that was there when we drafted him ... That's the way to throw the ball to Dez, I'll say that. You give him those kind of opportunities."
Hayes had 71 touchdown catches in 128 games with the Cowboys from 1965 to '74. Bryant has recorded his 72 touchdown catches in 109 games. Bryant also holds the team record for touchdown catches in a season with 16 in 2014.
In the season opener, Jason Witten set the franchise record for receiving yards, passing Hall of Famer Michael Irvin.