Six men will be charged over the importation of nearly $50 million of cocaine supplied by a Mexican drug cartel.
In pre-dawn raids on Tuesday, five men were arrested in a joint police operation sparked by the seizure of 188 kilos of the drug in 2019.
Another man, already in jail on drug charges, will be issued with a court attendance notice.
Border Force officials found the shipment concealed in hollowed out aluminium blocks imported from Mexico in February 2019.
The shipment amounts to up to 940,000 individual street deals of cocaine, and is estimated to be worth about $47 million.
The seizure helped police identified an Australian-based criminal syndicate allegedly behind multiple drug importations.
Another bust was made last December, with 50kg of ephedrine seized by Border Force in Sydney, and 50kg of iodine confiscated during two search warrants.
Almost 40kg of methamphetamine with an estimated street value of $9.5 million could have been made with the confiscated products, police say.
Two men implicated in the cocaine importation will also face charges relating to the December bust.
The five other men arrested, aged between 37 and 69, are expected to be charged with attempting to possess an unlawfully imported commercial quantity of cocaine.
They face life imprisonment.
NSW Police Drug and Firearm Squad Commander Detective Superintendent John Watson says the arrests are a big win for the police agencies working to stop the drug trade in Australia.
"The syndicate that has been brought down today is significant and shutting it down will put a substantial dent in the drug trade in NSW and across the country," he said.