After a near-perfect performance on day one which saw India bowled out for just 76 and England close the day on 120-0, Joe Root led the way on day two as his side pressed home their advantage.
Having both reached their half-centuries on day one, neither Rory Burns or Haseeb Hameed were able to go on and reach three figures.
Burns was the first to fall, getting bowled through the gate by Mohammed Shami for 61, before Hameed was bowled by Ravi Jadeja for 68.
Dawid Malan, in his first Test innings since 2018, then put on a 100-run partnership with captain Root as both players reached their half-centuries.
It marks the first time that every member of England's top four have passed 50 in the same innings since March 2013.
Malan eventually fell to the last ball before tea, getting caught down the legside for 70.
Root continued to score runs freely, reaching his 23rd Test century and sixth this year with a flick for four.
England then endured a lower order collapse, with four wickets falling for just 33 runs.
Jonny Bairstow was the first to go, getting by Virat Kohli for 29 and Jos Buttler soon followed for just seven.
Root's magnificent innings then finally came to an end after he was bowled by Jasprit Bumrah for 121, before Moeen Ali was caught for eight and Sam Curran was dismissed for 15.
Craig Overton and Ollie Robinson then saw England through to the close of play on 423-8 with a lead of 345 runs.
Here are five talking points from the day's play.
Hameed looks here to stay
Hameed may not have gone on to score a hundred in this Test, but his score of 68 marked a remarkable return to England fold after almost five years out in the wilderness.
Having had an impressive debut series in India in 2016, scoring 219 runs at an average of 43.80, injury problems and a stark drop off in form saw him leave Lancashire for Nottinghamshire in 2019 in a bid to kickstart his faltering career.
And the move did just that, earning Hameed a return to Test cricket and his first innings as an England opener since November 2016 suggested that he may well be here to stay.
Speaking on BBC Test Match Special, former England captain Michael Vaughan said: "He's played beautifully.
"He negated the early threat from India, looked very composed and confident at the crease. He's got England in a very good position and the game is moving on nicely."
Malan made his return to the England Test side after three years away, having dined almost exclusively on a diet of T20 cricket in that time.
The 33-year-old had played just one game of first-class cricket this year ahead of his return, scoring 199 for Yorkshire against a largely inexperienced Sussex attack in June.
Despite his lack of red ball cricket, Malan looked assured on his return, getting off the mark with an eye-catching cover drive, putting on a 139-run partnership with Root and scoring 70.
Speaking on BBC Test Match Special, former India wicketkeeper Deep Dasgupta said: "Dawid Malan is a great addition to this Test team.
"He has got a lot of runs in white-ball cricket and that is what this Test team needs at the moment – experience and confidence. I really like him because he has a compact game."
Root's golden form continues
For the first time in 13 Test matches, the England captain was afforded the opportunity of coming into bat with more than 100 runs already on the board thanks to Hameed and Burns' partnership.
And Root looked to make the most of that opportunity, racing to his half-century off just 57 balls as he played with great fluency.
Root had already scored two hundreds in this series and notched his third in double-quick time, breaking a number of records in the process before he was eventually dismissed for 121.
The 30-year-old is in a golden run of form at the moment we are privileged to be able to watch him at the peak of his powers.
Spin to win?
There has been an ongoing debate during this series about whether India should pick Ravichandran Ashwin as a second spinner.
Kohli has publicly stated that he prefers to have four seamers and Jadeja as his five-man attack in England, but there has been plenty of evidence that this pitch will spin as the game goes on.
Ali extracted some spin in his brief two-over spell on day one and Jadeja also found some turn.
Speaking on BBC Test Match Special, former England spinner Vic Marks said: "There would have been a case for Ravichandran Ashwin and Ravindra Jadeja in this India line-up because it really hasn't done much for the India seamers and it should spin as the game progresses."
Ishant Sharma has been a dependable performer for India in recent years, but the veteran seamer was not at his best at Headingley.
Sharma opened the bowling poorly on day one and he was surprisingly entrusted to open the bowling on day two ahead of Jasprit Bumrah.
The 32-year-old ended day two with figures of 0-92 from 22 overs and an economy rate of 4.18 and former India bowler Ajit Agarkar was particularly critical of his display.
"I think Ishant Sharma started with some nice, friendly deliveries outside off, exactly what India didn't need after getting only 78 runs on the board," Agarkar told Sony Sports.
"That's why you have to question why he was given the first over. I know he is the senior guy with a lot of experience.
"But at the moment, there are two guys who are better than him at the moment in the team."
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