Gill was 265 not out at tea on the second day, with his innings the cornerstone of India’s imposing 564-7.
The 25-year-old Gill, in just his second Test as captain, set a new record Thursday for the highest score by an India batsman in a Test in England, surpassing the great Sunil Gavaskar’s 221 at the Oval back in 1979.
Gill also received excellent support from spin-bowling all-rounders Ravindra Jadeja (89) and Washington Sundar in partnerships of 203 and 144 for the sixth and seventh wickets respectively.
Already a Test-best 168 not out at lunch, Gill continued to take a toll of England’s attack as he once more batted in near flawless fashion.
He was especially severe on Shoaib Bashir, cover-driving the off-spinner for four and lofting him for six.
Gill also struck two fours in three balls off fast bowler Josh Tongue, an on-drive followed by a flick off the hip that saw Joe Root and Zak Crawley almost collide in a failed attempt to prevent the boundary.
A hooked single off Tongue took Gill to 200 in 311 balls, including 21 fours and two sixes, wit the elated skipper bowing to a capacity crowd in celebration.
It was occasional off-spinner Root who took the lone wicket of the session when he bowled left-hander Sundar with a delivery that turned and bounced.
India, making fine use of a flat pitch, still scored 145-1 in the 31 overs between lunch and tea.
By that stage Gill had bettered his Test-best score for the second match in a row after making 147 in last week’s five-wicket loss at Headingley, where England went 1-0 up in a five-match series.
India, batting in ideal sunny conditions on Thursday, wanted even more runs from their sixth-wicket duo after collapses of 7-41 and 6-31 cost them dear at Headingley.
Jadeja went to 50 with a single off local hero Chris Woakes. Stokes introduced Bashir and set a 6-3 legside field for paceman Brydon Carse, with England trying increasingly unusual methods to make a breakthrough on a good batting pitch.
Gill’s single off Bashir took him to 150. Buoyed by setting a new personal best with the largest of his seven hundreds in 34 Tests, Gill then reverse-swept Bashir for four.
Jadeja lofted Bashir for six to bring up India’s 400 and Gill raised the sixth-wicket duo’s 200-run stand in style by slog-sweeping the spinner for another six.
But 10 minutes before lunch, Jadeja gloved a short ball from Tongue to wicketkeeper Jamie Smith. He faced 137 balls, striking 10 fours and a six.