Azaria Byrne, from Sydney band The Art, and his partner Brooke Mitchell were among nine people charged over alleged large-scale drug manufacture and supply following busts.
While searching the studio at Leichhardt in Sydney's inner-west on Wednesday, police dogs led officers to a wall gleaming with electric guitars.
A small push soon unveiled another door, which opened to a room allegedly containing ketamine, cannabis and other illicit drugs on an extraordinary scale.
The police haul allegedly uncovered more than 17kg of cannabis, 25kg of ketamine, 2.5kg of cocaine, 3.5kg of MDMA or ecstasy and 5.6kg of diazepam.
About 18,000 tablets believed to contain LSD, magic mushrooms, meth and $200,000 cash were also allegedly found.
Searches at Byrne and Mitchell's home in Earlwood, as well as others in North Bondi, Potts Point, Dulwich Hill and Marrickville revealed more wads of cash and a litany of other substances, police seizing drugs worth about $5.5 million.
One of the Marrickville properties was suspected to have been used as a drug laboratory after MDMA, ketamine and drug-making equipment was seized.
"Our detectives are tireless," Acting Superintendent Gretchen Atkins told reporters, noting police had been working on the matter since August.
"They will leave no stone unturned, they will keep going to identify people who are responsible for this, and take them and these drugs off the street."
Byrne, 45, and Mitchell, 28, were both refused bail and remanded for eight weeks after facing Burwood Local Court via video link on Thursday on dozens of drug supply charges.
The frontman faces 10 counts of the most serious charge - large commercial drug supply - while Mitchell faces one.
If convicted of those offences, the pair face a maximum term of life imprisonment.
Byrne was arrested wearing a shirt from Frankie's Pizza, a now-closed rock 'n' roll bar co-owned by The Art's drummer Jordan McDonald.
There is no suggestion McDonald or other band members were involved in the alleged drug operation.
The band had previously performed alongside Jimmy Barnes and taken the stage at other iconic Sydney venues like Crowbar in the inner west.
Alleged ringleader, Potts Point music producer Oliver Dibley, 33, did not apply for bail after facing an online bail court.
He is accused of knowingly directing the activities of a criminal group and 17 large commercial drug supply offences.
All three are due back in court on May 14.
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