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The 31-year-old Californian twins defeated American Eric Butorac and Jean-Julien Rojer of Netherland Antilles in just over an hour and a quarter.
The Bryans had been bidding for another page in the record books since claiming their 61st at the Madrid Masters in May. Their opponents on court at UCLA were playing their first event together.
Mark Woodforde, who lives two hours east in a California desert resort, was watching in the stands as his record with longtime partner Todd Woodbridge set a decade ago was broken.
"It means everything to have Mark here, it's awesome," said Mike Bryan. "We looked up to the Woodies, they were a class act. We learned from them, their technique was flawless, it was great to have a legend here today.
"This is an unbelievable record. To share this with my brother is everything."
Nearly 100 friends and family were among the crowd in the stands as the record was set.
"When you talk about 100 finals, that's a lot of Sundays, two years' worth. It's just amazing to believe how much work you put into each one of those," said Bob Bryan.
"There is no way I could have imagined this," said Bryan. "To get one of the Woodies record is special. I could barely hold the racket near the end I was so nervous."
Woodforde and Woodbridge were inducted into the International Tennis Hall of Fame three weeks ago in the US state of Rhode Island.
"For many years, you've been travelling in elite company," said Woodforde in the post-match trophy presentation, "Now you're in rare air, you stand alone as one.
"I can say that Todd and I wish you the very best. Our run ended when I elected to retire, but I'm sure the floodgates will open for you - 70-80 titles are quite possible."
The Bryans own a record six titles in LA, where they first got wildcards as teenagers. They had to wait for two and a half months to finally nose to the title after their last victory in Madrid was followed by a second round French Open defeat and a quarterfinal loss at Wimbledon.
