The visitors were 51-2 at tea on day two at the Melbourne Cricket Ground, still 423 runs adrift after the hosts were all out soon after lunch on the back of Smith’s dogged 140.
Yashasvi Jaiswal was not out 23, weathering a fiery blast from Australia’s pace attack, with KL Rahul bowled by Cummins for 24 on the cusp of the break.
Skipper Rohit reverted to his usual role as opener after dropping to six in the past two Tests.
But it did nothing to help his woeful recent form and he was out for three, spooning an attempted pull shot off the Australian captain to Boland at mid-on for a simple catch.
The hosts resumed on 311-6 after a dominant opening day where all their top four blasted 50 or more to lay a solid platform.
That thrilling action was also notable for Virat Kohli’s shoulder barge on debutant Sam Konstas, with the Indian superstar fined 20 percent of his match fee.
Australia plundered another 163 runs on Friday, with the composed Smith slamming 13 fours and three sixes.
Paceman Jasprit Bumrah took 4-99 and spinner Ravindra Jadeja 3-78.
Smith padded up again on 68, with Cummins alongside him on eight.
They took 15 off one Akash Deep over before Smith hooked Bumrah for six to rub salt in the wounds, with India’s body language showing their frustration.
Smith reached his 34th Test century with a boundary off Nitish Kumar Reddy, which came on the back of a return to form in the last Test in Brisbane where he made 101.
It was a patient innings from the 35-year-old and moved him alongside four other players on the all-time list of century-makers, including Sunil Gavaskar and Brian Lara.