Coming off scoring his first Test century since June 2023 in Brisbane, the resurgent veteran (68no) enters day two poised to make a fifth ton at the MCG.
If Smith can hit a 34th century, it will move Australia towards a potentially Test-winning total after going to stumps on day one at 6-311.
The 35-year-old seemed to be facing his cricketing mortality after making a combined 19 runs across the first two Tests.
It extended his drought without a Test century into 18 months.
But after 101 at the Gabba, Smith continued his late-career revival with some vintage form on Thursday.
It came after teenager Sam Konstas smashed an unforgettable 60 to begin his international career, bravely taking on India's strike weapon Jasprit Bumrah.
Usman Khawaja (57) and Marnus Labuschagne (72) also made starts, making it the first time Australia's top-four had all passed 50 in the same innings since the first Test in Pakistan in March 2022.
Australia captain Pat Cummins won his first toss of the series, electing to bat first to escape the sweltering conditions on Thursday when the temperature soared to 39C.
The MCG has become a bowler-friendly venue since Scott Boland's famous debut against England in 2021.
Only two totals of more than 300 have been posted across the three Boxing Day Tests prior to this one.
Superstar veteran Virat Kohli, who Konstas idolised growing up, is set to be sanctioned for his shoulder bump on the 19-year-old.
A villain of the Australian crowds this summer, India fast bowler Mohammed Siraj fired off words to Konstas multiple times.
Sam Konstas hit the third-quickest half-century by an Australian Test debutant on day one at the MCG (AP PHOTO)
"I was just trying to get in the contest and whoever I was facing, just trying to bring the best version of myself," Konstas said.
"Obviously it got a bit heated at times, which was good for me.
"Just feel like that brings the best out of me, and hopefully I go well next innings."
26°C