Helicopters, sniffer dogs and teams specializing in detecting bunkers and other hideaways joined the operation, they said.
It targeted 116 individuals from 24 crime families, sought for criminal association, extortion, fraud, illegal possession of arms and other offences.
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Based on tightly knit clans, the 'Ndrangheta has its stronghold in Calabria, the "toe" of Italy, although recent arrests have shown it is also operating in northern Italy and has expanded to other European countries.
It is widely believed to have outstripped the better-known Sicilian and Neapolitan mafias through its successful cocaine trafficking from Latin America.