Looking for a breakthrough win, the 36-year-old Thai dropped a bogey on the first hole but did not let it bog him down and sank six birdies, including three on the trot, to stay one shot ahead of Sri Lankan Mithun Perera.
"I didn't expect to be in the lead actually, having missed the halfway cuts two weeks in a row in Bangladesh and on the ADT (Asian Development Tour) in Malaysia last week," said Atthaphon.
"I played with an open mind. I didn't think much out there and I played solid. I drove the ball well and my putting was good."
Starting on the back nine, Perera was flawless with five birdies through 16 holes but slipped out of lead after dropping a shot on the eighth at the Santiburi Samui Country Club.
"I played good golf today but I thought I could be better as I missed the birdies on four to five holes, all from within five feet," Perera said after his best round in his three attempts at the Asian Tour event staged in honour of Thailand's Queen Sirikit.
Seven players, including 2009 winner Chinnarat Phadungsil of Thailand, India's Chiragh Kumar and Jeunghun Wang of Korea shared third place on 68.
Defending champion Thaworn Wiratchant of Thailand was among those bunched in 10th place a further one shot behind.
(Reporting by Amlan Chakraborty in New Delhi; editing by Sudipto Ganguly)
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