The federal opposition plans to introduce legislation to parliament in March that would punish anyone who helps the so-called "ISIS brides" return to Australia with up to 10 years' jail.
A group of 34 Australian women and children has been trying to return home from a Syrian refugee camp.
They travelled to the Middle East with men who wanted to fight for Islamic State before the terror organisation was defeated in 2019.
They have been issued with Australian passports but were unable to travel to the Syrian capital Damascus for a flight home.
Prime Minister Anthony Albanese was scathing of the coalition's proposal, describing it as "nonsense that was not thought through in order to get a headline".
"They themselves couldn't explain how that was constitutional," he told ABC radio on Tuesday.
He reiterated the government would not be repatriating the group and temporary exclusion laws were already operating.
One of the women has been barred from returning after being handed a temporary exclusion order under Australian counterterrorism laws.
"The full force of the law has been implemented to the extent that we can," Mr Albanese said.
Opposition Leader Angus Taylor said he would make it illegal to help the repatriation of people who had travelled to declared terrorist hotspots or committed a terrorist offence.
"We need to shut the door to people who are going to bring hate and violence to our shores from another part of the world," he said on Monday.
Greens home affairs spokesperson David Shoebridge slammed the coalition for proposing non-government organisations like Save the Children Australia be criminalised for helping Australians return home.
"The idea that any serious Australian political party would make it a crime for Australians to try and help Australian children and bring them back to safety is a remarkable low, even in the current climate on the immigration debate," the senator told ABC radio.
Save the Children Australia chief executive Mat Tinkle said the proposed laws sounded like a "reckless" thought bubble that would set a dangerous precedent.
"I think it's pretty reckless, to be honest," he told ABC TV on Monday.
Mr Tinkler said he did not know whether his organisation would be caught up in the coalition's policy and has offered to brief the party on Save the Children's work in Syria.
Mr Albanese doubled down on his remarks that he is sympathetic with the children stuck in Syria, but that it was a choice made by their parents to go there.
The prime minister's assertion on Monday that the coalition allowed more than 40 people into Australia, including fighters, was rejected by former leader Scott Morrison who said only orphaned minors were granted entry under his government.
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