The American drawcard will start Saturday's second round at The Grange two shots shy of leader Sam Horsfield.
Horsfield's bogey-free six-under 66 has the 28-year-old Englishman dreaming of what could be "the best (win) of my pro career".
"These fields are very, very strong," Horsfield said.
"And the thing of it is, everyone plays aggressively so you're always going to have guys that go out there and shoot low."
Horsfield is one stroke ahead of Chile's Joaquin Niemann and Mexico's Carlos Ortiz.
DeChambeau and Dustin Johnson sit at four under with fellow major winners Brooks Koepka (three under), Jon Rahm and Bubba Watson (both two under) also contending.
But Australians Lucas Herbert (one under), Cam Smith (even par), Marc Leishman (one over) and Matt Jones (three over) need to make a second-round move.
The big-hitting DeChambeau can potentially reach some of The Grange's par-4s with one trademark drive but said patience would be key to his chances.
"It's really wind dependent," DeChambeau said.
"If I get a good wind and I can hit it up by the green and there's not much trouble up around the green, I'm going to go for it.
"It's really being patient on these par-4s and deciding what is going to give me the best opportunity to make birdie on the hole.
"It's a risk-reward thing. You can't get too far ahead of yourself."
Renowned as a left-field thinker and a constant tinkerer with technique and technology, the reigning US Open champion said he felt "really, really close" to his ultimate goal.
"Every time I tee it up, I want to win," he said.
"Last year everybody said: 'Oh, you're just focused on the majors'.
"Well, no, I was focused every time I went out and played a golf tournament.
"But what I'm really looking for is a golf swing that is just a little bit more consistent and repeatable.
"I'm getting close. I'm getting really, really close.
"What I had at the US Open was pretty darned good ... (I) want to get back to that form.
"But I'm still searching for what I did so well at Greenbrier back in late '23 when I shot 58. That was the best I'd ever hit the golf ball.
"I'm always striving to get back to that place and just trying to learn what was it that exactly clicked in that manner."
DeChambeau became the fourth player on a top-level tour to shoot 58 when winning his maiden LIV Golf title in West Virginia in August 2023.