England bowled out India for 329 in 48.2 overs after attacking half-centuries from Rishabh Pant and Hardik Pandya in the deciding third one-day international on Sunday.
Pace bowler Mark Wood claimed three wickets while leg-spinner Adil Rashid took two after England opted to bowl in the decider in Pune.
England need 330 to clinch the series at a venue where they chased down 337 in the previous ODI to go level 1-1.
Pant top-scored with 78 and Hardik smashed 64 after India were in trouble at 157-4.
India started strongly with a 103-run opening stand between Rohit Sharma and Shikhar Dhawan before Rashid removed the openers.
Rashid bowled Sharma for 37 on a googly and then took a return catch in his next over to send back the left-handed Dhawan out for 67.
Moeen Ali soon combined forces to rattle the stumps of Virat Kohli as the dejected batsman walked back in his 200th international as India captain.
Liam Livingstone picked up a wicket on his second ball to send back previous game centurion KL Rahul for five.
Pant and Hardik counter-attacked with a flurry of boundaries as India crossed the 200-run mark inside 30 overs.
The left-handed Pant swatted a six off Rashid to bring up his second successive half-century and kept up the attack with Hardik.
Pant, who hit four sixes in his 62-ball knock, finally fell to Sam Curran with captain and wicketkeeper Jos Buttler taking a low sharp catch to break the 99-run stand.
Hardik reached his fifty in 36 balls after he was joined by elder brother Krunal Pandya, who had hit an unbeaten half-century on debut in India's opening win.
Shardul Thakur hit 30 off 21 balls but India lost their final four wickets for eight runs as Wood struck thrice including two in one over.