India's Ravindra Jadeja took the big wicket of captain Steve Smith to damage Australia's hopes of salvaging a draw on the final day of the third Test in Ranchi on Monday.
Australia were 83 for four at lunch with Shaun Marsh on 15 and Peter Handscomb on four, needing another 69 runs to avoid an innings defeat.
Quick bowler Ishant Sharma got the first breakthrough when he trapped Matt Renshaw plumb in front for 15 with a delivery that kept low.
But it was Smith's wicket off the left-arm spin of Jadeja that created the loudest noise at India's newest Test venue.
Smith was on 21 when he tried to pad away a viciously turning delivery from Jadeja that spun from outside leg to rattle the right-handed batsman's off stump.
Smith, who scored an unbeaten 178 in the first innings, resisted for 68 balls second time around before Jadeja's exploitation of the rough created by the bowlers' footmarks paid off.
It was the third wicket of the innings for Jadeja, who had also removed vice-captain and opening batsman David Warner for 14 and night watchman Nathan Lyon for two late on day four.
Renshaw and Smith survived the first hour of play with some sensible batting during their 36-run third-wicket stand until the pressure exerted by India caught up with the visitors.
Virat Kohli's side had seized control of the match on Sunday after declaring their first innings on 603 for nine, a lead of 152 runs.
Cheteshwar Pujara with 202 and Wriddhiman Saha, who scored 117, shared a 199-run partnership for the seventh wicket to script India's turnaround in response to Australia's 451.
The four-match series for the Border-Gavaskar Trophy is tied 1-1.