More arrests may be made as the investigation progresses, police say.
A total of 127 people were targeted in Operation Loquace. Of those people, 26 are still at large.
Sûreté du Québec officials say 10 other arrests were made without warrants during Thursday's raids.
Six people were allegedly leading the criminal activities and relying on other organizations to import and distribute large amounts of cocaine, police said.
Two of the alleged leaders, identified as Shane Maloney and Larry Amero, were apprehended in Montreal's Verdun borough and face charges of of conspiracy to traffic drugs, drug trafficking, conspiracy to import drugs, drug importation and gangsterism.
Amero is allegedly linked to the Hell's Angels in British Columbia.
Maloney was arrested in June after an off-duty Montreal police officer was beaten up in Playa del Carmen, Mexico.
A news release issued by the provincial police earlier on Thursday identifies some of the 111 people arrested as important members of the Hells Angels and the Italian Mafia, but no further details were given.
The warrants were executed in Quebec and Ontario, according to Sgt. Grégory Gomez Del Prado of Quebec provincial police. B.C. police are also involved in the investigation.
Twenty-two police forces teamed up to carry out search warrants in 30 municipalities in Quebec this morning in connection with the crackdown on organized crime and the drug trade.
The SQ's vice-director Jean Audette said "the consortium did not hesitate to use violence to spread its market. Many parallel cases are being investigated in Quebec and elsewhere in the country."
According to authorities, members of the Hells Angels and other participants in organized crime were partnering to import and distribute large amounts of cocaine.
A police news release says a total of $255,000 in cash, 6,000 pills, nine kilograms of cannabis, three kilograms of cocaine, 13 barrels of GBL (a solvent used in creating date rape drugs) and 35 vehicles were seized in today's operation.
Police also seized five residences with a total estimated value of $1.5 million.
Before today, police seized 153 kilograms of cocaine and 46,100 units of methamphetamines, along with 161 guns, 291 prohibited weapons, 1,486 explosives and 50 detonators in a sweep connected to the latest raids.
Distribution related to the Mexican drug cartel
A separate operation that took place in Sainte-Sophie in August yielded nearly 400 guns, other weapons and several stolen explosives that were hidden in a warehouse.
Audette said the police estimate the organization could distribute up to 75 kilograms of cocaine in the span of a week.
Police said the drug network was closely affiliated with the Mexican drug cartel and used ground transit to bring cocaine to Canada.
Authorities said the network's worth was estimated at $50 million after six months of drug distribution.
Police mentioned some of the people arrested were linked to violent crimes, but would not divulge more details.
The alleged leader of the cocaine trafficking operation was arrested in a residential complex on Montreal's Nun's Island this morning, according to Radio-Canada.
Nearly 1,000 police officers from Quebec services and the RCMP are involved in the ongoing investigation.
Police in Laval, Que. said 20 warrants were executed on their territory since 6:30 a.m. ET. Around 70 of their officers were involved, including two tactical teams.
At the Montreal police's northern operational building, streams of marked and unmarked police cars carrying suspects arrived throughout the morning
Memories of biker raids
Police likened the scale of Thursday's operation to their last two massive ones targeting bikers in Quebec.
"It's a very large operation – we're talking about one almost as large as the ones we made in [operations] Springtime and SharQC," said Sgt. Benoit Richard of the provincial police.
Operation SharQC, carried out in Quebec and New Brunswick in 2009, targeted the Hells Angels and led to the arrest of 111 full-patch members of the club. Thirteen members arrested in the sweep pleaded guilty this spring to charges of murder and conspiracy to commit murder.
The 2001 Operation Springtime also targeted the Hells Angels and led to the arrest of dozens of club members and associates and further charges laid against former president of the Montreal chapter, Maurice (Mom) Boucher.