The raids were the culmination of an investigation code named Pollino that was launched in 2016 against the 'Ndrangheta criminal group on allegations of cocaine trafficking, money laundering, bribery and violence, said Eurojust, the European prosecution agency that fights cross-border organized crime, which co-ordinated the operation.
A total of 84 suspects were arrested as police in Italy, Germany, Belgium, Holland and Luxembourg raided the homes of suspected mafia bosses and searched restaurants and other businesses early yesterday morning.
It has surpassed Sicily's Cosa Nostra and the Naples-based Camorra in influence thanks to control of the cocaine trade and is the sole mafia organisation to operate on all continents, according to anti-mafia prosecutors.
Germany's Federal Criminal Police Office (BKA) also said raids had been carried out on the Spanish island of Mallorca.
He said the "unprecedented and extraordinary result" 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 worldwide drug trafficking, Italian police said in a statement.
Italy's anti-mafia prosecutor Federico Cafiero De Raho said Wednesday's operation was just a "first step" and the group had not yet been defeated.
In Germany, the raids - which are part of Operation Pollino - are focused on the western state of North Rhine-Westphalia, where the mafia has traditionally had a large presence. His arrest was among the 46 people taken into custody.
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The Mafia group hails from Calabria, the region that forms the tip of Italy's boot, and has made substantial inroads in European countries.
"We send a clear message to organised crime groups across Europe".
Italian restaurants and ice cream parlours used to launder money were among the premises raided.
'Ndrangheta is one of five major world crime organizations operating out of Italy.
Wednesday's raids come a day after the new suspected head of the Cosa Nostra and 45 other alleged gangsters were arrested.
Dutch NOS television said the 'Ndrangheta were mainly active in the Netherlands in drug smuggling through the country's huge flower export market.
Jeweller Mineo, 80, was detained with at least 45 others just before he was due to be appointed official heir to notorious mafia boss Toto Riina, who died in prison a year ago.