Alleged senior Alameddine gang member Masood Zakaria was arrested when he landed in Darwin on Sunday afternoon.
NSW Police Assistant Commissioner Michael Fitzgerald described the 28-year-old as one of the state's "most wanted and significant" organised-crime figures.
Zakaria has been a focus of a transnational offshore task force, known as Operation Gain, targeting the nation's most prominent overseas-based offenders.
The Sydney man was wanted by police over his claimed links to the Alameddine gang and his alleged involvement in a failed plot to murder underworld figure Ibrahem Hamze.
Police thwarted an alleged attempt to kill Hamze in 2021 when they tried to stop a stolen Mercedes in North Sydney that investigators say was to be used for the crime.
Several men have already been charged with conspiring to murder Hamze.
Assistant Commissioner Michael Fitzgerald described Zakaria as a "significant" crime figure in NSW. (Steven Saphore/AAP PHOTOS)
Mr Fitzgerald said Zakaria fled Australia in a fishing boat as police were about to arrest him in 2022.
"We believe that he fled to Western Australia and got on a fishing boat and travelled overseas where he eventually landed in Turkey," he said.
Police believed Zakaria was second in charge of one of Sydney's largest crime gangs, Mr Fitzgerald added.
Turkish officials notified Australian authorities after Zakaria allegedly entered the country in 2022 on a false passport.
Further inquiries established he was living in the city of Bodrum, on the country's southwest coast.
While overseas, police said Zakaria continued to associate with a number of organised crime figures with significant Australian links.
He was arrested and transferred to immigration detention by Turkish authorities in January and has been held in custody awaiting deportation.
Since arriving in Darwin on Sunday, Zakaria has been held on a NSW arrest warrant for offences including conspiracy to murder, knowingly directing the activities of a criminal group, supplying a large commercial quantity of cocaine and dealing in the proceeds of crime.
Several of the offences carry maximum jail terms of life in prison.
Australian Federal Police Assistant Commissioner Stephen Dametto said Australians who hid offshore in perceived safe havens to avoid facing court, would be caught.Â
"More than 70 per cent of the transnational serious organised criminals who target Australia are offshore," he said in a statement on Monday.
"One by one, these alleged criminals are being extradited or deported to Australia to face the justice system."
Zakaria is scheduled to face Darwin Magistrates Court later on Monday, when NSW Police will make an application to extradite him.
