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.
Operation Pollino was co-ordinated by Eurojust, the EU's cross-border justice authority, which described it as a "decisive" intervention against organised crime.
In Germany, federal police said there had been multiple arrests in the early morning raids. Around 90 arrests were made; 4,000 kilograms (8,820 pounds) of cocaine and 140 kilograms of ecstasy pills were seized.
The group has links with drug cartels in Colombia and Mexico, Italian anti-Mafia prosecutor Federico Cafiero de Raho said in The Hague.
"Today we send a clear message to organized crime groups across Europe", said Filippo Spiezia, vice president of Eurojust, the European Union prosecution agency that coordinated the raids.
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".
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The crackdown on the powerful organised crime syndicate based in Calabria, southern Italy, came just a day after Italian police arrested the new boss of the Cosa Nostra Sicilian mafia and dozens of other suspects in a major operation.
In Germany, Wednesday's operation focused on restaurants, offices and apartments linked to the mafia group, focused on the North Rhine-Westphalia region, Der Spiegel reported. They are accused of committing "serious crimes" including activities linked to worldwide drug trafficking, Italian police said in a statement.
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.
On Tuesday, Italian police arrested new Cosa Nostra boss Settimino Mineo and dozens of other suspects in Sicily.
Some 2 million euros (2.3 million dollars) in criminal assets was seized, Eurojust Vice-President Filippo Spiezia said in The Hague.
In Germany, the raids constituted the country's greatest strike against the mafia, arresting 14 suspects.
The 'Ndrangheta is considered the leading mafia group that managed to extend its reach even amid the scrutiny and constant arrests.