The American has yet to record a victory on either the DP World Tour or the PGA TOUR but has so far come closest in golf's four biggest events.
The 25-year-old has played in seven Majors in his career, with four top-tens including a second-placed finish at the 2021 Masters Tournament.
After carding his best Major round on day one with a 66, he went one better to get to nine under and lead the way from Chile's Mito Pereira, who carded a 64.
American Justin Thomas played in the tougher side of the draw and he mastered the wind in the morning with a 67 to sit at six under, a shot clear of countryman Bubba Watson who signed for a remarkable 63 with nine birdies.
Zalatoris finished 14th in the DP World Tour Rankings in Partnership with Rolex in his rookie season last year and is now looking for a first win on the biggest stage, with his only previous professional victory being on the Korn Ferry Tour in 2020.
"They're tough golf courses, that allows my ball-striking to really give me the best chances," he said of his performances in Major Championships. "Obviously these greens aren't easy but hitting them on the right tiers and being able to have the 15-25-footers where I'm not going up and down slopes is huge.
"The other part too, I think, is just I've kind of had an attitude with the Majors. I don't want to leave anything, looking back 20 years from now I don't want to regret my attitude or anything like that.
"So I just make sure that after every single shot I hit, it's just, I don't want to say life or death but make sure I'm fully committed to everything that I do because we only get four of them a year.
"I've got a long 36 holes ahead of me. I think if anything you're able to plot your way around this golf course and, if you hit as many greens as you possibly can, it's kind of hard to mess it up.
I don't want to leave anything, looking back 20 years from now I don't want to regret my attitude or anything like that
"If you get on the wrong slopes it still has a little bit of the attitude of like Augusta where you can hit 18 greens and walk off that place and shoot 80.
"I think history to me, it is what it is, but I'm going to go out and do my job and hopefully it's enough at the end."
With high winds in the morning, Thomas was highly impressive as he carded four birdies and a bogey to set the target but with conditions calmer in the afternoon, both Zalatoris and Pereira moved past him.
Zalatoris recovered from a ragged tee-shot on the first to make a birdie and after a run of nine pars, he put his tee-shot on the 11th to five feet to join Thomas at the summit.
Pereira hold from around ten feet on the tenth and 11th and while he gave a shot back on the 12th, he holed a 20-footer on the 16th, and then was dialled back in on the second and fourth to join the lead.
Zalatoris put approaches inside ten feet at the 12th and 13th but Pereira was relentless and after taking advantage of the par-five fifth, he hit another fine shot into the seventh.
It looked like he could lead on his own when Zalatoris hit another poor tee-shot on the 17th but a brilliant second and a seven-foot putt gave the Californian the lead.
McIlroy made a single birdie on the 12th after recording two bogeys on the front nine, while Ancer carded three birdies and two bogeys and Riley also made three gains with a single blemish.