With his double century in sight, the 25-year-old Trinidadian smashed a Jake Ball full delivery against his ankle off an inside edge in the 46th over and dropped to the ground twisting in agony.
He was then wheeled away on a stretcher to a standing ovation.
His career-best haul, off 130 balls, included seven sixes and surpassed the previous international record for a retired hurt of 165 set by Australian Charles Bannerman against England in 1877.
West Indies ended the innings on 356 for 5 off 50 overs, leaving England a huge total to chase and giving the visitors a chance of remaining in contention to draw the series on Friday.
England, who have an unbeatable 2-0 lead after winning the third game by 124 runs in Bristol last Sunday, were without Ben Stokes and Alex Hales after both were involved in a nightclub incident on Monday.
Stokes was earlier named in England's Ashes squad for the tour of Australia.
(Reporting by Alan Baldwin, editing by Toby Davis)
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