More than a tonne of the drug - worth over $1.8 billion - was allegedly ferried to customers in specially modified cars by a group known as The Commission over a four-month period.
The syndicate's clients included several other crime networks carving out their own slice of Sydney's lucrative cocaine market, police said.
A group of men arrested in raids across the city on Wednesday claimed to be part of The Commission, a storied alliance said to dominate the local drug trade.
But unlike others arrested in the past, the latest cohort claiming affiliation with the syndicate are believed to be telling the truth.
"I've been a part of a lot of major investigations in relation to drugs where people claim to be a part of The Commission - and that's generally lies," Detective Superintendent Peter Faux said on Thursday.
"But the methodology, where these people were clearly dictating the amount of cocaine hitting the streets ... their professionalism and the complexities around this crew is all consistent with being a part of The Commission," he said.
Wannabe kingpins often claimed affiliation with the syndicate to create a "fear factor" in rivals, Det Supt Faux added.
More than $55 million worth of drugs were seized as part of the operation, although that paled into comparison with the estimated $1.8 billion the group allegedly shipped across NSW between February and July.
Police say the syndicate directly controlled the supply and price of cocaine in Sydney, a national hotspot for consumption of the drug.
The product was routinely stashed inside hidden compartments in cars for transport, while those involved in the transaction minimised face-to-face contact in order to keep their identities secret.
NSW Police Commissioner Karen Webb said other criminals considering stepping in to take control of the drugs trade should think again.
"Our actions yesterday and over the last 12 months show NSW Police is eradicating serious threats to NSW and Australia time and time again," she said.
The arrest of a man in July set police on the trail of a coke gang, resulting in multiple seizures. (Supplied/AAP PHOTOS)
NSW Police began an operation with secretive state and national crime commissions in July, when a 21-year-old man from Sydney's west was charged with commercial drug supply.
He was also charged with dealing with proceeds of crime and participating in a criminal group.
The initial arrest put investigators on the trail of other participants in The Commission.
Officers seized 20kg of cocaine, found in a bag thrown over a fence, on Wednesday morning.
Ten cars, $800,000 in cash, a Rolex watch, guns, "homemade" ballistic vests and electronic devices were also seized during the raids across southwest Sydney.
The otherwise ordinary cars had been modified with sophisticated hiding places, including one that held up to 10kg of cocaine, Det Supt Faux said.
The syndicate was rigidly structured and subtle.
"They would never be seen by the people that they were actually supplying the drugs to, which was quite unique," Det Supt Faux added.
Officers also found packets of drugs hidden in a number of cars. (HANDOUT/NSW POLICE)
Six men were arrested and charged with drug supply and criminal group offences following the raids.
The group's 25-year-old alleged director was refused bail when he faced court on Wednesday.
Five others will appear on Thursday.
