Luggage was allegedly used to carry 33 kilograms of methylamphetamine onboard the Indian Pacific Train to Perth at the weekend.
A 25-year-old NSW man and a 27-year-old Victorian man were arrested as they left the East Perth train station on Saturday during a joint operation by West Australian Police and the Australian Criminal Intelligence Commission.
Detective Superintendent Kim Massam said the seizure, which is estimated to be worth $33 million, was equal to 330,000 hits of the drug in the community.
"These jobs are now become very long, ongoing investigations into working out where the source of the drug came from and where it was going to," he told reporters on Monday.
"We are absolute in our resolve to chase down the people behind this criminal enterprise and put them in jail."
The men have been charged with possessing a trafficable quantity of meth with intent to sell, plus other charges.
They appeared in court on Sunday and are scheduled to appear in Perth Magistrates Court on August 22.
More than 1.4 tonnes of meth has been seized so far this year, Det Supt Massam said.