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.
A total of 84 suspects were arrested as police in Italy, Germany, Belgium, the Netherlands and Luxembourg raided the homes of suspected mafia bosses and searched restaurants and other businesses in the early hours of the morning.
It has approximately 6,000 members, and is believed to control 80-percent of Europe's cocaine trade.
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", the fruit of a two-year operation, targeted "dangerous members of the 'Ndrangheta family deeply involved in drug trafficking and money laundering".
Italian police said 90 people had so far been detained.
Giovanni Bombardieri, an Italian prosecutor, said that "sophisticated investigative techniques" were used to monitor the crime group's operations and communications, and characterized the violence linked to 'Ndrangheta as tantamount to "carnage".
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"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. His arrest was among the 46 people taken into custody. The focus was on the western state of North Rhine-Westphalia, which borders the Netherlands and Belgium, and Bavaria to the south.
Officials hailed Wednesday's operation - dubbed "Operation Pollina" - as a serious blow to the group.
The European police agency Europol said it was a "decisive hit against one of the most powerful Italian criminal networks in the world".
He added, groups of the 'Ndrangheta and its allies, have infiltrated the ports around Europe and "polluted" lawyers and accountants in many countries on their payrolls.
Dutch outlet NOS said that the 'Ndrangheta is known to operate its drug smuggling through the country's vibrant flower-trading industry.
The raids came a day after Italian police arrested Settimo Mineo, the new head of Sicily's Cosa Nostra mafia.
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.