Immigration officials detained 34-year-old Luke Joshua Cook and his Thai wife Kanyarat Wedphitak at Bangkok's main airport on Saturday for attempting to smuggle half a tonne of crystal meth into Thailand in 2015.
Cook is accused of trying to bring the drugs to land from a boat moored in the Gulf of Thailand. He was spooked by a patrol boat and threw a large amount of the "ice" overboard.
Cook's arrest comes amid a widening crackdown against the Hells Angels, who have chapters based in Bangkok and Pattaya, a Thai resort notorious for its seedy nightlife and criminal networks.
Police conducted raids on the motorcycle gang's residences and businesses in Pattaya last week and on Sunday, seizing money, property, vehicles and guns.
"It is a big transnational crime organisation which is just escalating its operations in Thailand," Major General Apichat Sirisith told reporters on Tuesday as police revealed Cook's arrest.
With roots in the US, the Hells Angels spread to other countries, establishing chapters around the world.
Their Pattaya chapter grabbed headlines in early 2015 when an Australian Hells Angel leader was found dead after being kidnapped by masked men.
Earlier this year, Australian national Antonio Bagnato, 28, was convicted of the murder of a Wayne Schneider earlier this year and sentenced to death, a verdict rarely carried out in Thailand.
Schneider was once on an Australian "most wanted" list for shooting a bouncer in the knee outside a Sydney nightclub.
Both moved to Thailand and chose to live in Pattaya.
Cook is believed to have helped the Bagnato escape to Cambodia where he was later arrested, Thai police said.
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