Bart Allen Helmus and his Thai wife Sirinapha Wiset-rit have been arrested at a property in Sa Kaeo.
Thai media reported Helmus allegedly shot himself as officers swooped in.
He has been taken to hospital.
Earlier, Noi or Ton Nilthes, who was the other suspect to escape from Pattaya Court on Monday was recaptured.
Police said they apprehended Nilthes in Sa Kaeo province close to the border with Cambodia.
A video shared on Facebook purportedly showed Nilthes being led away by police.
Earlier on Wednesday multiple Thai news outlets reported that Sirinapha Wiset-rit, 30, had been arrested on Tuesday night.
However, by mid-morning Wednesday contradictory reports in Thai media said she was still on the run along with her American husband.
On Tuesday police described the three suspects as dangerous and warned the public not to approach them.
On Tuesday afternoon the getaway vehicle used by the group was found abandoned in Sri Racha, while a white Mitsubishi car also thought to be used by the group was found in Sa Kaeo on Tuesday night.
It was initially believed the white Mitsubishi was used by Sirinapha Wiset-rit and it was the discovery of this vehicle that lead to reports of her arrest, but that was not the case.
On Monday, Helmus, Sirinapha and Nilthes were due to face drugs charges in Pattaya Provincial Court.
The American and his wife were arrested in Pattaya in July after being found in possession of nearly 1kg of crystal meth, a pistol and 200 bullets.
However, before the hearing they escaped after Helmus stabbed a guard at the court while Nilthes, who was armed with a gun, forced guards to hand over the keys to their ankle chains.
They fled to a waiting Isuzu pick up truck.
A huge manhunt was then put in place, with police stating from the outset they believed the trio would try to head for the border with Cambodia.
An investigation is underway to establish how Helmus and Nilthes came to be in possession of a knife and gun.
This is a developing news story. This post may be updated without warning.Facebook.
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