Day 2 at Lord's began with England resuming on 21/1, looking to erase India's first-innings advantage.
England lost early wickets, but Amy Jones (52) and Nat Sciver-Brunt rebuilt with a 99-run partnership, taking the score to 131/5.
Sciver-Brunt fell with 142 on the board before Kranti Gaud claimed the first-ever Women's Test five-wicket haul at Lord's.
England's tail added valuable runs, but were eventually bowled out for 170, conceding a 115-run first-innings lead.
India began positively in the second innings as Shafali Verma struck a composed 33 off 55 balls, helping them to 78/1.
Smriti Mandhana remained unbeaten on 69, registering back-to-back Test fifties, while Yastika Bhatia added a solid 39*.
Sophie Ecclestone claimed India's only wicket of the innings, dismissing Shafali Verma.
At stumps, India were 154/1, leading by 269 runs with nine wickets in hand and two days remaining.