The intercepted haul destined for European markets is thought to be worth around €100m.
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Portuguese authorities announced on Tuesday they had seized 4.2 tonnes of cocaine hidden in pallets of bananas from Colombia.
This is "the biggest cocaine seizure this year and one of the biggest in recent years", said Vitor Ananias, criminal investigation coordinator at the Judiciary Police.
The drugs, concealed in six pallets filled with bananas, entered Portuguese territory on board a cargo ship flying the Italian flag through the port of Setubal, 30km south of Lisbon.
According to police, the drug was "of a high degree of purity". Ananias said it was "destined for several European countries" and estimated its value to be "more than €100 million".
The authorities say the seizure will do "heavy financial damage" to criminal organisations distributing the drug around Europe.
The operation to intercept the shipment was the result of international cooperation with Colombia and several European countries.
No one has been arrested as yet.
It comes a week after Italian police found two tonnes of cocaine floating in waterproof packages in the sea near Sicily, possibly after being dropped off a cargo ship for collection later.
That haul was thought to be worth around €400 million, and is one of the largest single seizures by Italian authorities in almost three decades.