Australians who travel to the heartland of terror group Islamic State in Syria without legitimate cause face up to 10 years in jail.
In the first declaration under new counter-terror laws designed to deter terrorist tourism, the province of Al-Raqqa has been deemed off limits.
Foreign Minister Julie Bishop says the government is determined to stop Australians from supporting and engaging in hostile activities with listed terrorist organisations.
"Declaring Al-Raqqa province under the criminal code sends a strong message to those Australians who seek to participate in the Syrian conflict," she said.
Ms Bishop is considering declaring additional areas where Islamic State (ISIL) is engaging in hostile activities.
Previously, Australians could travel to such conflict zones but, in the absence of any evidence of wrongdoing, they committed no offence under Australian law.
There are provisions to exempt people with a legitimate reason for going there, including journalists.
It is part of measures aimed at keeping Australian ISIL supporters out of Syria and Iraq and minimising the risk of returned jihadists launching terror attacks.
Already 75 Australians believed to be in Syria and Iraq have had their passports cancelled. The government has refused to issue passports to another 10 planning to travel to the region.
In Al-Raqqa, the minister said, ISIL is murdering opponents, raping and enslaving women and intimidating and subjugating the civilian population to their brutal control.
"It is one of the world's most deadly and active terrorist organisations and has been listed as a terrorist organisation in Australia under its various names since 2005," she said.
Some 60 Australians are believed to be fighting with Islamist terror groups in Syria and Iraq, with the UN estimating about 200 foreign fighters join ISIL every month.
Labor backed this move on Thursday, but not the Greens.
Opposition deputy leader Tanya Plibersek said Labor was pleased to support this extraordinary measure of declaring a whole area a no-go zone.
"We are very concerned about the increasing numbers of Australians going to this region and the broader region to fight," she said.
Greens Senator Penny Wright said the draconian move could catch innocent Australians overseas, criminalising legitimate travel.
"Anyone who travels to the Al Raqqa province, even under the listed exemptions, will have a very real legal challenge of proving that they went there for one sole purpose," she said in a statement.
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