An eight-month investigation by Victoria Police alleges the group imported more than 11kg of methylamphetamine from Spain and 2.8 million illegal cigarettes from Dubai, both of which have been seized by officers.
The police also discovered 14 firearms, a stolen car, a boat, luxury jewellery and designer clothes.
In March and April, the Australian Border Force (ABF) detected several packages which were allegedly sent using international freight to factories in Craigieburn and Epping, and a storage facility in Flemington.
Victoria Police had already launched an investigation into the group's alleged trafficking of firearms and drugs across the state but began investigating the group's import activity after receiving ABF's reports.
Six people from northern suburbs of Melbourne were arrested on May 7, facing a range of drug trafficking offences.
On Tuesday, two of the syndicate - a 32-year-old man and 25-year-old woman - were landed with a combined 100 further charges, and the man was also charged with 26 counts of breaching parole.
All six will appear at Melbourne Magistrates' Court on September 30.
The investigation is ongoing and seven other people were arrested in July and August, including an 18-year-old man and 58-year-old woman who were interviewed and released pending further inquiries.
Detective Inspector Geoff Owen from North West Metro Regional Crime Squad says officers are determined to make Victoria a "hostile place for organised crime".
"We can only imagine the harm caused if these drugs and firearms made their way into the community."
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