With the prospect of a hung parliament still looming, Shorten said that Turnbull should resign because he cannot command his own party and the Australian voters have concluded he is "out of touch".
"This is farcical. Turnbull clearly doesn't know what he is doing. Quite frankly I think he should quit," Shorten, 49, said.
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"This guy is like David Cameron of the southern hemisphere," he said.
"He leads a divided party, he has had an election and he has delivered an inferior and unstable outcome."
"He has taken this nation to an election on the basis of stability. He has delivered instability."
"His own party knows he is not up to the job, the Australian people know he is out of touch and he has given a Senate reform which involves two or three One Nation senators."
A confident Labor leader said he would work to deliver the stability Turnbull promised repeatedly at the election, by reaching out collaboratively to the crossbenchers in the new parliament.
Shorten also said the prime minister had made a bad situation worse with Senate reforms.
Shorten's decision to up the ante against the prime minister comes as internal recriminations about the poor election showing continue within the Coalition. Senator Nick Xenophon is positioning himself as the new parliamentary kingmaker, signalling he is prepared to enter some form of minority government agreement with either Turnbull or Shorten.
Meanwhile, it is still not clear which party will form government after Saturday's vote.
Shorten upped the ante against 61-year-old Turnbull, as the poor election showing continue within the Coalition, and Nick Xenophon is positioning himself as the new parliamentary kingmaker.
According to the latest update from Australian Electoral Commission, Labor had 71 seats while Turnbull-led Liberal/National Coalition has 67. Counting will resume on Tuesday.
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