After India were bowled out for 499 in their first innings replying to Australia's 408, India skipper Mahendra Singh Dhoni pressed the attack button from the word go as Australia came out to bat in Sunday's last session.
Dhoni's trick worked as medium pacer Bhuvneshwar Kumar rattled the top order with his swinging deliveries, taking all the three wickets.
Resuming the day at 283/0, India's debutant Shikhar Dhawan (187) could add only two more runs in the morning to his record breaking knock, falling 13 short of a double century.
Dhawan Saturday scored the fastest ton (85 balls) on debut in recorded cricketing history. His 187 is also the highest by an Indian debutant and sixth highest in the world.
Murali Vijay (152), who played a mere support role to Dhawan on the third day, anchored the Indian innings Sunday scoring his third Test century in the process and second of the series. His innings included 19 splendid boundaries and three huge sixes.
Batting great Sachin Tendulkar (37) provided good support to Vijay before falling to leg spinner Steven Smith. After the exit of Vijay and Tendulkar, the lower order did not contribute much barring Virat Kohli, who remained unbeaten on 67.
Fast bowler Peter Siddle was the pick of the bowlers for Australia as he clinched the seventh five-wicket haul of his career (5/71). Left arm pacer Mitchel Starc also provided the important breakthroughs of Vijay and Dhoni (4), leading to the slide of the Indian batting order.
Moises Henriques, Nathan Lyon and Smith took a wicket each to bowl out India, who ended with a lead of 91 runs.
In reply, Bhuvneshwar provided another superb spell of swing bowling on a dry and flat fourth day wicket to dismiss the three Australian wickets to fall, the first one coming on the third ball of the second innings.
Only Phillip Hughes stood out among the Australian batsmen as David Warner (2), Ed Cowan (8) and Smith (5) walked back to the pavilion almost as quickly as they came out of it.
At stumps, Hughes and nightwatchman Lyon were batting at 53 and 4, respectively.
Australia's in-form skipper Michael Clarke, who batted at No.3 in the first innings, had a sore back and did not come out to bat. There is speculation he might not bat Monday either which will give the home side an even better chance to take an unassailable 3-0 lead going into the fourth and final Test in New Delhi beginning March 22.
Australia (First innings) 408
India (First innings, overnight 283/0)
Murali Vijay lbw b Starc 153
Shikhar Dhawan c Cowan b Lyon 187
Cheteshwar Pujara lbw b Siddle 1
Sachin Tendulkar c Cowan b Smith 37
Virat Kohli not out 67
Mahendra Singh Dhoni lbw b Starc 4
Ravindra Jadeja c Haddin b Siddle 8
Ravichandran Ashwin c Haddin b Siddle 4
Bhuvneshwar Kumar c Haddin b Henriques 18
Ishant Sharma c Haddin b Siddle 0
Pragyan Ojha b Siddle 1
Extras (b 5, lb 13, nb 1) 19
Total: (all out in 132.1 overs) 499
Fall of wickets: 1-289 (Dhawan, 59.5 overs), 2-292 (Pujara, 62.6), 3-384 (Tendulkar, 94.1), 4-412 (Vijay, 101.1), 5-416 (Dhoni, 101.4), 6-427 (Jadeja, 104.5), 7-431 (Ashwin, 106.5), 8-492 (Kumar, 129.6), 9-493 (Sharma, 130.6), 10-499 (Ojha, 132.1)
Mitchell Starc 23-5-74-2
Peter Siddle 29.1-9-71-5
Moises Henriques 15-1-62-1
Nathan Lyon 31-4-124-1
Xavier Doherty 24-8-87-0
Steven Smith 10-0-63-1
Australia (2nd innings)
David Warner c Dhoni b Kumar 2
Ed Cowan lbw b Kumar 8
Phil Hughes batting 53
Steven Smith b Kumar 5
Nathan Lyon batting 4
Extras (lb 2, nb 1) 3
Total (for three wickets in 21 overs) 75
Fall of wickets: 1-2 (Warner, 0.3 overs), 2-35 (Cowan, 7.5), 3-55 (Smith, 13.5)
Bhuvneshwar Kumar 8-1-25-3
Ishant Sharma 2-0-11-0
Ravichandran Ashwin 7-2-25-0
Ravindra Jadeja 2-1-11-0
Pragyan Ojha 2-1-1-0
Test debut: Shikhar Dhawan (India)
Umpires: Aleem Dar (Pakistan) and R.A. Kettleborough (England)
TV umpire: S. Asnani
Match referee: R.S. Madugalle (Sri Lanka)
Reserve umpire: R.M. Deshpande