The global sweep involved police in Germany, Italy, the Netherlands and Belgium working together against the powerful organised crime syndicate based in southern Italy.
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.
Authorities in the Netherlands, Italy, Germany, Belgium and Luxembourg worked together on the operation with the code name "Pollino", coordinated by the Eurojust from 2016, assisted by Europol.
Authorities said they conducted raids in Germany, Italy, Belgium and the Netherlands in a crackdown on the 'Ndrangheta, a southern Italy-based organized crime group.
Officials said by midday of the operation, nearly 4,000 kilos of cocaine and hundreds of kilos of other drugs were seized. Cocaine and ecstasy pills also were seized in Wednesday's raids.
It is the only mafia organisation operating on all continents, say prosecutors, and is believed to now be the most influential Italian organised-crime group.
Italian police said the sweep targeted the 'Ndrangheta and its "projections across South America".
The Mafia group hails from Calabria, the region that forms the tip of Italy's boot, and has made substantial inroads in European countries.
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Some 2 million euros (2.3 million dollars) in criminal assets was seized, Eurojust Vice-President Filippo Spiezia said in The Hague.
'Ndrangheta is thought to control as much as 80 percent of the cocaine trade in Europe, according to the BBC, and boasts around 6,000 members.
In Germany, the raids constituted the country's greatest strike against the mafia, arresting 14 suspects.
Wednesday's raids come a day after the new suspected head of the Cosa Nostra and 45 other alleged gangsters were arrested.
The Belgian operations were concentrated on the Limburg area, home to many people of Italian descent who moved there after World War II to work in coal mines, Belgian prosecutors said.
But Italy's top Mafia prosecutor, Federico Cafiero De Raho, also sounded a note of caution, saying the raids only scratched the surface of the powerful 'ndrangheta, whose tentacles and illicit activities, including huge cocaine trafficking operations, were spread all over the world.
In Germany, the operation focused on restaurants, offices and apartments, mainly in the states of North Rhine-Westphalia and Bavaria, with 21 suspects targeted.
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