Authorities in Germany, Italy, Belgium and the Netherlands launched coordinated raids Wednesday in a crackdown on the Italian mafia.
Wednesday's raids were the culmination of a two-year investigation codenamed Pollino against the powerful 'ndrangheta criminal group on allegations of cocaine trafficking, money laundering, bribery and violence, Eurojust said.
Eurojust, the European Union agency that coordinates cross-border crime fighting, announced the raids in a statement.
More than 80 people with suspected links to the 'Ndrangheta Mafia - considered one of the world's largest organized crime groups - have been arrested during raids in six European countries and in the South American country of Suriname.
Dutch chief public prosecutor Fred Westerbeke said dozens of raids also netted about 2 million euros (£1.7 million) in criminal proceeds as well as drugs including ecstasy and cocaine.
Italian police said 90 people had been arrested so far in the operation targeting the 'Ndrangheta group and its "projections across South America".
He said the "unprecedented and extraordinary result" targeted "dangerous members of the 'Ndrangheta family deeply involved in drug trafficking and money laundering".
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On Tuesday, Italian police arrested new Cosa Nostra boss Settimino Mineo and dozens of other suspects in Sicily in a major swoop.
But he warned that it was "just a first step", saying the arrests were "nothing for the 'Ndrangheta, there are thousands of people who should be arrested and billions that should be seized".
The group surpassed Sicily's Cosa Nostra and the Naples-based Camorra groups, according to AFP, due to its tight on the control of cocaine trade.
In Germany, the operation focused on restaurants, offices and apartments, mainly in the states of North Rhine-Westphalia and Bavaria, with 21 suspects targeted.
"It's nearly a cliche, but the operation carried out today confirms again the great danger of the 'ndrangheta, not just in drug trafficking, where it's the undisputed leader, but (also) in the financial sphere", said Francesco Ratta, a top police official in the southern Italian region of Calabria.
In Germany, 14 arrests were made, German prosecutor Horst Bien said.
"They are invisible", Cafiero de Raho added.
The 'ndrangheta "is the most important organized crime group in the world", said Gen. Alessandro Barbera, who commands the investigative unit of Italy's financial police corps.