Hundreds of police are understood to have been involved in the operation in Belgium, Italy, Germany and the Netherlands.
"Today, supported by a coordination center at Eurojust, judicial and law enforcement authorities from the Netherlands, Italy, Germany and Belgium are now executing arrests and seizures against a 'Ndrangheta criminal group involved in cocaine trafficking, money laundering, bribery and violence", Wednesday's statement read.
In Germany, federal police said there had been multiple arrests in the early morning raids on premises linked to the southern Italy-based organized crime group. Most raids took place in the western state of North Rhine Westphalia, but also in the south, in Bavaria.
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.
"Today, we send a clear message to organised crime groups across Europe".
The 'Ndrangheta is seen as the most powerful Italian mafia organization, and a leading force in money laundering and the cocaine trade.
Officials hailed Wednesday's operation - dubbed "Operation Pollina" - as a serious blow to the group.
Dutch chief public prosecutor Fred Westerbeke said dozens of raids also netted about 2 million euros (£1.7 million) in criminal proceeds as well as drugs including ecstasy and cocaine.
The 'Ndrangheta, centered in the Calabria region, is one of Italy's three main organised crime groups, along with the Camorra, which is based in the Naples area, and Sicily's Cosa Nostra, commonly known as the Mafia.
Two arrests were made in Luxembourg, and five in the Netherlands, Eurojust said. "There are thousands of people who should be arrested and billions of euros that should be seized".
Italian anti-mafia prosecutor Federico Cafiero De Raho said the operations would affect the 'Ndrangheta's drug trafficking operations around the world, including in Colombia, Ecuador, and Brazil.
On Tuesday, Italian police arrested an alleged Sicilian mafia boss, Settimino Mineo, believed to be the new head of the Cosa Nostra clan.
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 past year.