After being dismissed for a duck in the first innings, the 22-year-old star has piled serious pain onto Australia, as India moved to 1-275 at lunch on day three of the first Border-Gavaskar Test at Optus Stadium.
India lead by 321 runs, and will try to make Australia field all day in the Perth sun, with the temperature expected to reach 35 degrees.
Jaiswal (141*) and KL Rahul (77), who was only recalled to the Indian team because captain Rohit Sharma was on parental leave, put on a 201-run stand - the highest opening partnership by an Indian pair in Australia.
The duo eclipsed the previous mark of 191, set by Sunil Gavaskar and Kris Srikkanth at the SCG in 1986.
Jaiswal, who grew up in the slums of India, reached his fourth Test century early on Sunday when he ramped Josh Hazlewood over fine leg for six.
The left-hander triumphantly raised his hands in the air before hugging Rahul.
Jaiswal has made life a hot and steamy misery for Australia, with 12 fours and three sixes. (Dean Lewins/AAP PHOTOS)
Despite two Test centuries in India and another away to the struggling West Indies, doubts had lingered over how Jaiswal would perform in Australian conditions.
But he has excelled on a pace-friendly Perth pitch that has admittedly become easier to bat on after 17 wickets tumbled on a chaotic opening day.
Jaiswal went to lunch alongside Devdutt Padikkal (25*), who also made a first-innings duck and is playing only his second Test.Â
With Australia heading towards their first Test defeat at Optus Stadium since it opened in 2018, and just their second overall in Perth against India, Pat Cummins' team will have to defy history.
The last time Australia recovered from a 1-0 deficit and came back to win a Test series was in the 1997 Ashes in England.
Australia last won a Border-Gavaskar series in 2014-15, with India holding the trophy since 2017.
This has been a stunning turnaround for India, who arrived in Australia fresh off a historic 3-0 home whitewash at the hands of New Zealand.
Mitchell Starc (1-79) has taken Australia's only wicket of the innings, looking frustrated even after removing Rahul when the Indian right-hander was caught behind.
Even taking the second new ball just before lunch failed to help Australia make any serious inroads.
The Aussies were skittled for a woeful 104 in their first-innings, replaying to India's 150, after stand-in captain Jasprit Bumrah (5-30) bowled superbly to enhance his already stellar reputation in Australia.
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