Tasmanian Senator Jacqui Lambie says the opposition needs to tell Scott Morrison to resign immediately over revelations he gave himself five secret portfolios.
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However former Nationals leader Barnaby Joyce said the former prime minister has not done anything illegal and there are concerns about setting a precedent.
It comes as it is now revealed ASIO was also kept in the dark that Mr Morrison secretly appointed himself as joint minister in health, finance, treasury, home affairs and the industry, science and resources portfolios.
Prime Minister Anthony Albanese has described the revelations as "weird" and as an "unprecedented trashing of our democracy", while ordering the Solicitor-General to investigate further and report back over the affair on Monday.
Liberal frontbencher Karen Andrews is leading the Coalition voices calling for Mr Morrison to resign, although The Canberra Times has spoken to another senior Coalition figure urging him to leave as soon as possible so the Liberals can move forward as a party.
Senator Lambie is urging the Liberal party to tap Mr Morrison on the shoulder.
"He needs to be told," she told RN Breakfast on Wednesday.
"You cannot just close your eyes on this and allow him to just walk around like he's still a member of Parliament ... It's time for him to go. It's time for Scott Morrison to resign. Enough damage has been done already."
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The former prime minister has apologised, in a long Facebook post, to colleagues who have been offended by his actions, although he did not explain the need for secrecy.
Senator Lambie said public trust in politicians is very low and the revelations surrounding Mr Morrison are not helping.
"I can tell you, unless they start to gather themselves together and start standing together as one, they are going to become non-existent, whether they would hear that this morning or not, but that is where you are heading," she said.
But while investigations continue, former Nationals leader Barnaby Joyce has stated Mr Morrison has not broken any law or has done anything illegal.
"Improper? Well, that's a question to take up with Mr Morrison. But illegal? No," he said.
"Do I think it is the right thing to do? No, it's not. Why? Because we have a cabinet system of government. We do not have a presidential system of government."
Mr Joyce indicated the concern was around setting a precedent.
"Well, gee whiz, if you're gonna use that as the test, let's make sure we stick to this term of government and anytime there's something improper, will immediately ask for someone's head on a spike," he told the ABC.
"Even the Labor Party wouldn't agree to that one."
The one time Mr Morrison used his extra powers was to override then resources minister Keith Pitt to reject the gas exploration permit for the PEP-11 to be granted off the NSW coast.
Mr Joyce insists Mr Pitt should have made the decision, not the then prime minister.
"It should not have been Scott Morrison, it should have been Keith Pitt," he said.
Meantime, Home Affairs Minister Clare O'Neil has confirmed the chief of ASIO, Mike Burgess, did not know Morrison was the minister for home affairs for a significant period of government.
"If you don't understand how vulnerable that made us, you should not be in parliament," she said.
Ms O'Neil also said there is no confidence that Mr Morrison did not make decisions as home affairs minister.