Members of French Gendarmerie, Europol and Guardia Civil taking part in a joint operation against smugglers. AFP
Operation Dark HunTOR also recovered millions of euros in cash and bitcoin, as well as drugs and guns. The bust stems from a German-led police sting earlier this year taking down the "world's largest" darknet marketplace.
Dark HunTOR, "was composed of a series of separate but complementary actions in Australia, Bulgaria, France, Germany, Italy, the Netherlands, Switzerland, the United Kingdom, and the United States," the Hague-based Europol said.
In the United States alone, police arrested 65 people, while 47 were held in Germany, 24 in Britain, and four each in Italy and the Netherlands, among others.
A number of those arrested "were considered high-value targets" by Europol.
Law agents also confiscated 26.7 million euros ($31 million) in cash and virtual currencies, as well as 45 guns and 234 kilogrammes (516 pounds) of drugs, including 25,000 ecstasy pills.
Italian police also shut down the "DeepSea" and "Berlusconi" marketplaces, "which together boasted over 100,000 announcements of illegal products", said Europol, which coordinated the operation together with its twin judicial agency Eurojust.
German police in January closed down the "DarkMarket" online marketplace, used by its alleged operator, an Australian, to facilitate the sale of drugs, stolen credit card data and malware.
'Trove of evidence'
Europol said the arrest of the alleged operator, caught near the German-Danish border at the time, and the seizure of the criminal infrastructure provided "investigators across the world with a trove of evidence".
German prosecutors at the time said DarkMarket came to light in the course of a major investigation against the web-hosting service Cyberbunker, located in a former NATO bunker in southwest Germany.
Europol's European Cybercrime Centre EC3 has since been compiling intelligence packages to identify the key targets, the continent's policing agency said.
The secret "darknet" includes websites that can be assessed only with specific software or authorisations, ensuring anonymity for users.
They have faced increased pressure from international law enforcement in recent months.
"The point of operations such as this is to put criminals operating on the dark web on notice (that) the law enforcement community has the means and global partnerships to unmask them and hold them accountable for their illegal activities," Europol deputy director of operations Jean-Philippe Lecouffe said.
Rolf van Wegberg, cybercrime investigator at the TU Delft university said the operation signalled a break in the trend of recent police actions against suspected online criminals.
"This kind of operations in the past looked at arresting the controllers of these marketplaces, we now see police services targeting the top sellers," he told investigative journalists at the Dutch KRO-NCRV public broadcaster.