Though he rued a missed birdie opportunity at the par-three eighth, his penultimate hole, Day picked up five shots over the closing stretch to become just the fifth player to card a 63 at the event widely regarded as the unofficial fifth major.
"I played solid from tee to green and I was very confident with my putter," Day told Golf Channel after finishing two ahead of Americans Cameron Tringale, Bill Haas and Brendan Steele, England's Justin Rose and Ireland's Shane Lowry.
"Just got things going. Unfortunately it didn't go in on eight," he said of a narrow miss with a 40-foot putt at the eighth that would have given him a birdie-birdie-birdie finish.
"I really wanted to hole that putt to then try and give myself a birdie on nine to beat the record but I will take tying the course record."
Fred Couples in 1992 was the first player to shoot 63 at the TPC Sawgrass before Greg Norman (1994), Roberto Castro (2013), Martin Kaymer (2014) and then Day followed suit.
PGA Championship winner Day, who has long coveted a first Players title to add to his already impressive golfing resume, felt that fatigue had helped his on-course focus.
"It's been a long week because it's been hot and I just felt really tired for some reason," said the 28-year-old Australian, who has won six tournaments in his last 16 starts. "That kind of distracted me from anything else.
"The scores here are so low. When you shoot a nine-under-par round, you expect - especially on this course - to have a decent lead. I've got only a two-shot lead and there's a slew of guys that are at seven under and at six and five (under)."
Four-times major winner Ernie Els of South Africa, Italy's Francesco Molinari and Americans Hudson Swafford, Brooks Koepka, Daniel Berger and Boo Weekley opened with 66s while world number two Jordan Spieth double-bogeyed his final hole for a 72.
The late starters had to cope with strengthening winds in the afternoon when scoring became a little more difficult as American Rickie Fowler, the defending champion, and Northern Irish world number three Rory McIlroy both opened with 72s.
(Reporting by Mark Lamport-Stokes in Los Angeles; Editing by Larry Fine and Frank Pingue)
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