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Police arrested 45-year-old Scott Miller and a second, 47-year-old man on Tuesday morning after finding methylamphetamine concealed in eight candles in January.
Police say there was half a kilo of meth in each candle with the street value exceeding $2 million.
Police raided homes at Rozelle and Balmain and a business in Bankstown at dawn on Tuesday.
The two men were arrested with drugs and cash allegedly found at both homes. Police are still searching Miller's Rozelle home in Sydney's inner west.
Miller would be charged with directing a criminal syndicate and the other man with participating in a criminal syndicate, Detective Superintendent John Watson said on Tuesday.
Both will also be charged with supplying large commercial quantities of meth.
"It's alleged he's the director of this particular syndicate ... Others, it will be alleged, are working under his instruction," Supt Watson said.
The men were distributing drugs from Sydney that were bound for regional NSW. The eight candles were destined for Albury on the Victorian border.
"This was not a small operation," Supt Watson said.
"They were well organised and well financed. They were well set up and they were intent on delivering death and misery right through the state and in this case, Albury."
Police anticipate more arrests.
The concealment of the meth was sophisticated, with the drugs moulded into glass mouldings inside the candles. The meth had "very high purity", Supt Watson said.
Both men were surprised at the raids but now co-operating with police after being taken to Newtown Police Station, Supt Watson said.
The two men have a longstanding relationship.
Miller won silver and bronze at the 1996 Atlanta Olympics and was briefly married to Sydney model Charlotte Dawson.
Both accused are expected to face Newtown Local Court on Tuesday.