Nearly 400 officers spent the day conducting raids in Montreal, Laval and other municipalities in the area.
Laval police spokesman Sgt. Frederic Jean said in an interview that 36 warrants led to at least 42 arrests and the seizure of about 600,000 synthetic drug pills.
Investigators also confiscated nine weapons.
"Almost all of them were residential homes and one of them was a cottage," Jean said.
One of the homes in the Laurentians allegedly served as a transformation centre where equipment was used to turn powder into pill form.
Jean said two hydraulic presses were found as well as 100 kilograms of methamphetamine powder which had not yet been pressed into pills.
"It was a residential building that was actually used as a warehouse — as a stash for the purposes of this group," Jean said.
Jean said the network was a very well-structured group that had ties with the Italian Mob, the Hells Angels and street gangs.
Those arrested ranged in age from 21 all the way up to their 60s.
They will appear in court Wednesday to face a long list of charges that include drug possession, drug trafficking and possession with the intent to traffic.
Some of those arrested will also face charges related to weapons possession.
Jean described the crackdown as an important operation because young people are often targeted.
"Usually these drugs are taken by a younger crowd, adolescents and younger adults," he noted.
"The vast clientele really have no idea of the health risks they take when they take these drugs."
Jean said $300,000 in cash was also seized, as well as four ounces of cocaine.
In 2010 and 2011, the Laval drug squad seized an average 40,000 illegal pills per year and another 105,000 in 2012.
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