He posted a 17-under 196 total with one round remaining, while joint halfway leader Russell Knox of Scotland carded 66 for second place on 15 under.
Jimmy Walker vaulted into contention with a 62 to trail by four strokes, tied for third with Andrew Svoboda (67).
Tour rookie Andrew Putnam, who shared the halfway lead, shot 73 to plunge nine strokes off the pace.
Martin, 27, has not won in 55 starts on tour, but finished third three times last year.
“I want to win multiple times in my career and you’ve got to start somewhere,” the former U.S. Amateur runner-up told Golf Channel after securing the first 54-hole lead of his career.
“I’ve been playing well the last three days and (today) was just one of those days when you get in the zone.
“It felt like every single (yardage) was just the perfect number for whatever club I was hitting and I made the (putts) I was supposed to make and rolled a few more in. Everything went well.”
If Martin was spectacular, Knox was solid and he had no complaints about his performance.
"Bogey-free on a Saturday is a job well done," he said.
"I look forward to giving it a whack tomorrow. It's tough to win these tournaments. That's why I've never done it before.
"I'm going to hit bad shots tomorrow, but the second I get down on myself, I'm going to struggle, so I need to stand tall, smile as much as I can and really be like a pro."
Walker, a three-time winner last year, is the only player among the top four with a victory on tour.
He made a few minor tweaks to his swing pre-tournament under the guidance of coach Butch Harmon, and the work appears to be paying off.
“I didn’t drive it as well as I would have liked to on Thursday,” he said. “Yesterday was a little better and today it all felt pretty good.”
(Reporting By Andrew Both in Cary, North Carolina; Editing by Peter Rutherford)
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