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His girlfriend, Melbourne woman Antonietta Mannella, 28, has been arrested and taken into AFP headquarters.
Police say Ms Manella was George Marrogi’s link to the outside world.
“We will allege (Ms Manella) was carrying out his orders,” AFP assistant commissioner Krissy Barrett said.
The 33-year-old convicted murderer has been accused of plotting a sophisticated organised crime gang from inside the maximum security Barwon Prison.
The pair has also been charged with the importation of 56 kilograms of methamphetamine and 13 kilos of heroin in February.
The drugs were disguised in a shipment of green tea and magnets from Thailand.
Daily police phone taps allegedly uncovered plans for Marrogi to break out of prison, discussions of bashings and kidnappings, while also managing the proceeds of crime.
Police allege the pair weren’t working alone.
Two other people allegedly linked to the crime syndicate were arrested yesterday after raids at Point Cook, Greenvale and Gladstone Park.
A 32-year-old Point Cook man is expected to be charged with drug trafficking, and a 43-year-old Gladstone Park man faces drug possession charges.
Mr Marrogi faces drug importation charges as well as the charge for directing a criminal organisation, which carries a jail term of 15 years.
An additional charge of attempting to import 400 kilograms of methamphetamine was laid against Ms Manella on Monday.
Assistant Commissioner Barrett said the 456 kilograms of methamphetamine alone could have had a street value of $160 million.
“The harm is these drugs could have of caused if they reached our communities can not be overstated,” she said.
“We never give up when it comes to identifying the heads of criminal gangs and bringing them to justice.”
Detectives from Victoria’s Echo Taskforce also arrested two more men on Saturday, who were questioned over a conspiracy to murder, as part of an ongoing investigation into the large-scale organised crime syndicate.
A 31-year-old from Ringwood North was remanded in custody, while a 27-year-old from Mickleham was released pending further inquiries.
The arrests came after police said they received information that members of the syndicate –including people now in prison – were actively planning to kill several people.
Victoria Police said the Echo Taskforce had made 27 arrests linked to the gang’s activities and seized more than $2 million, luxury vehicles, and illicit drugs.
Police said the investigations into the threats to kill and other activities of the gang remain ongoing.
Ms Manella and Marrogi will face court again in August, while Marrogi will be sentenced for murder on Friday.