That left Langer two ahead of Americans Bill Glasson (64) and Doug Garwood (67), with Ireland's Mark McNulty (66) and Americans Joe Durant (68), John Riegger (64) and Michael Allen (64) a further stroke back at eight under.
Langer, however, dominated a mainly sunny day at Fox Chapel where his only cause of concern was a broken driver after he had teed off at the par-five last.
"I hit a good tee shot and as I picked up my tee, I heard it rattle in my driver head," Langer, a twice former Masters champion, told reporters. "And I'm going, 'Wow, what's that rattling for?'
"Then I grabbed the head, and it was loose. Something broke inside the screw that holds the shaft in. I have to go and see the tour rep down there or the guy that repairs the clubs and see if he can fix that one or I have to go to my backup driver."
Overall, though, Langer was delighted with his form on a day when his playing partner, reigning champion Kenny Perry, piled up seven birdies in a flawless 63 to surge into a tie for eighth at seven under.
"I saw Kenny Perry go low so I figured if him and I go low, there's going to be others that could go low too," smiled Langer, whose previous major wins on the Champions Tour came at the 2010 Senior Open Championship and the 2010 U.S. Senior Open.
"So I am trying to keep making the best shots I can and make more birdies."
Perry, who clinched his first over-50s major title with a closing 64 in last year's Senior Players Championship, accepts Langer will be difficult to beat over the weekend at Fox Chapel.
"I don't know if they're going to be able to fix that driver so it may give us a shot," Perry jested. "(Langer's) playing flawless golf. The only reason he made bogey on that 14th hole, he had a mud ball that shot it way left of the green.
"He's hitting it perfect, so he's going to be a hard man to catch. I'm going to have to keep shooting 63s to catch him."
Briton Colin Montgomerie, who won the Senior PGA Championship by four strokes in May, carded a 69 and was nine strokes off the pace.
(Reporting by Mark Lamport-Stokes in Los Angeles; Editing by Greg Stutchbury)
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