Australia face a battle to save the third Test after two Ravindra Jadeja wickets late on day four put India in a commanding position.
A double century from Cheteshwar Pujara and a hundred for Wriddhiman Saha had helped earn India a vital 152-run lead after the first innings as they declared on 603-9 in Ranchi.
That left Australia eight overs to bat out the day but after Jadeja bowled David Warner (14) and the nightwatchman Nathan Lyon (2), the visitors closed on 23-2.
India began day four on 360-6 with Pujara and Saha at the crease and there they remained until after tea, by that stage having taken their side past Australia's first innings total of 451.
Saha needed just one run in the evening session to go to his third Test century and duly got it before, after an incredible 521 deliveries, Pujara reached 200.
The stand ended at 199 as Pujara (202) chipped the ball to midwicket, looking to up the run rate, and Saha (117) fell to Steven O'Keefe (3-199) soon after.
Australia's frustration continued though as Jadeja (54no from 55 balls) made a swift half-century to extend India's lead and take their total past 600 before the declaration came.
After a quick turnaround, Jadeja (2-6) was back into the action and causing more trouble for the tourists, this time with the ball; his two wickets leaving Australia rocking with another 129 runs needed to make India bat again and facing a fight to salvage a draw on day five.
Watch day five of the the third Test between India and Australia from 3.50am on Monday, Sky Sports 2.