The suspected mafioso are believed to be involved in cocaine trafficking, money laundering, violence and bribery, said Eurojust, the European Union agency that coordinates cross-border crime fighting.
In an investigation that underscored an Italian crime syndicate's role as a leading player in worldwide cocaine trafficking, police in four countries arrested at least 84 suspected mobsters Wednesday in a series of carefully coordinated raids.
The 'Ndrangheta, a mafia organisation that operates out of the Calabria region of southern Italy, is one of the largest crime syndicates in the world, and is thought to make billions of pounds through cocaine trafficking every year.
He said the "unprecedented and extraordinary result", the fruit of a two-year operation, targeted "dangerous members of the 'Ndrangheta family deeply involved in drug trafficking and money laundering". They are accused of committing "serious crimes" including activities linked to global drug trafficking, Italian police said in a statement.
Italian prosecutor Federico Cafiero de Raho told reporters on Monday that he expects an ongoing investigation into 'Ndrangheta and that what the arrests made so far are "nothing to them".
German prosecutors said 65 premises linked to the southern Italy-based organised crime group were also being searched. "There are thousands of people who should be arrested and billions of euros that should be seized".
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Officials hailed Wednesday's operation - dubbed "Operation Pollina" - as a serious blow to the group.
Eurojust, the EU's Judicial Cooperation Unit, is a unit established to fight cross-border organized crime in Europe. The focus was on the western state of North Rhine-Westphalia, which borders the Netherlands and Belgium, and Bavaria to the south.
He added, groups of the 'Ndrangheta and its allies, have infiltrated the ports around Europe and "polluted" lawyers and accountants in many countries on their payrolls.
The Wednesday arrests came just a day after the authorities announced the arrest of Settimo Mineo, 80, the presumed new boss of the Cosa Nostra.
Five suspects were arrested in the Netherlands, where prosecutors got the ball rolling for the investigation in 2014 with probes into two Italian restaurants, and more suspects were detained just over the border in Belgium.
A 2012 police report showed the Ndrangheta could have as many as a hundred active members in this country.