Police launched a string of anti-mafia raids on Wednesday, targeting the notorious criminal franchise in Italy, Belgium, Germany, and the Netherlands, according to authorities.
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.
German federal police confirmed in a statement there had been multiple arrests in the early morning raids, with the main focus of the operation in western state of North Rhine-Westphalia, which borders Holland and Belgium.
It said the operation codenamed "Pollino" followed an investigation that began in 2016, adding that it would give more details at a press conference in The Hague later.
Police arrested dozens of suspected mobsters in Europe and South America on Wednesday in a huge global swoop targeting Italy's notorious 'Ndrangheta mafia clan, officials said.
But Federico Cafiero De Raho, Italian anti-mafia and anti-terrorism national prosecutor, sounded a note of caution, saying the raids only scratched the surface of the powerful 'Ndrangheta, whose tentacles and illicit activities spread all over the world.
Italian police arrested Settimo Mineo, 80, Tuesday, who authorities believe to be the lead Mafia boss who replaced the late Salvatore Riina.
The "Ndrangheta is seen as the most powerful Italian mafia organization, trumping Sicily's Cosa Nostra and Naples" Camorra.
Germany's Der Spiegel said 65 premises were being searched, including restaurants, apartments and offices, while Belgian media reported that arrests there were concentrated in eastern Limburg province. More than three tons of cocaine and about 300 pounds of ecstasy were seized.
Eurojust said those detained are suspected of drug trafficking, money laundering, bribery, and violence.
Two people were also arrested in Luxembourg, and one in Suriname.
The European police agency Europol said it was a "decisive hit against one of the most powerful Italian criminal networks in the world".
"Today we send a clear message to organized crime groups across Europe", Eurojust Vice-President Filippo Spiezia said.
Police swooped just a day after the alleged "godfather" of the Sicilian mafia was arrested, along with 45 other suspected mobsters.
Jeweller Mineo, 80, was detained along 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 previous year.