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Pant scored his first half-century of the series after Pujara was dismissed for a mammoth 193 runs, facing 373 balls and hitting 22 fours.
At the break, Pant was unbeaten on 88 runs, while Ravindra Jadeja was batting on 25 not out.
Post lunch, there were no signs of India speeding up the run-rate in order to declare quickly as the two batsmen batted as resolutely as in the morning.
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Pujara got a life on 192 when Usman Khawaja dropped him at slip off Nathan Lyon (3-144) in the 126th over.
But the batsman couldn’t score his first overseas Test double hundred and offered a tired return catch to Lyon four overs later.
He walked off to a standing ovation from the SCG ground, as Jadeja took guard.
The new partnership was also slow off the blocks scoring at just about 3 runs per over for the first eight overs.
But they slowly changed gears after Pant had reached his third Test half-century off 85 balls.
He shared 73 off 96 balls for the unbeaten seventh wicket with Jadeja, as the Australian bowlers looked tired and listless.
Earlier, India reached 389-5 at lunch.
Starting from overnight 303-4, Pujara took his fifth-wicket partnership with Hanuma Vihari (42) to 101 runs.
The duo came out with the intent to grind down the Australian bowling attack and looked content with batting for time.
However, Vihari’s hard work went to waste when he was caught at short leg off Lyon in the 102nd over.
There was the faintest blip on snickometer and the decision stayed in Australia’s favour despite Vihari’s quick DRS review.
Pant, on 8, had a loud shot for caught behind turned down in the 106th over as Tim Paine called for a DRS review. But there was nothing and he batted on.
From there onwards, the duo put on a chanceless partnership to dash Australian hopes further.
At the other end, Pujara batted solidly as ever and reached his 150 off 282 balls. His slow grinding partnership with Vihari meant that only 32 runs came off the first hour of play.
But he and Pant upped the ante in the second hour, adding another 54 runs later in the session.
Pujara crossed few milestones during this morning session. Firstly, he went past 153, his previous highest overseas Test score, against both South Africa (Johannesburg, 2013) and Sri Lanka (Galle, 2017).
He also became only the third Indian batsman to score 500-plus runs in a Test series against Australia, after Rahul Dravid in 2003-04 and Virat Kohli in 2014-15.
In doing so, he also batted 1200-plus deliveries thus far in the four matches, the most for an Indian batsman against Australia in a Test series, ahead of Dravid’s 1203 balls faced in 2003-04.
Pujara had finished day one on 130 not out, his 18th Test hundred and third century of this on-going series.
India have an unassailable 2-1 series’ lead after winning the first Test in Adelaide by 31 runs and the third Test in Melbourne by 137 runs. Australia had won the second Test in Perth by 146 runs.