Australia managed to steady their innings in the evening session following an onslaught from India's bowlers to close day one of the fourth and final Test on 231-8.
The visitors started strongly in Delhi by reaching 94-2, but were dealt a heavy blow in the afternoon session when they lost four wickets and were put on the back foot on 153-7.
The day belonged to Ravichandran Ashwin, who finished on a four-wicket haul, which included the dismissals of Ed Cowan (38), Steven Smith (46), Matthew Wade (2) and Mitchell Johnson (3).
Shane Watson returned to the squad following his axe from the third Test to take the captaincy role from injured Michael Clarke.
The all-rounder struggled to push up his nation's run-rate and was dismissed from the crease after just 17 runs by Ravindra Jadeja.
India have an unassailable 3-0 lead in the series.