Chanderpaul, officially the world's best batsman, fell shortly before tea on the fourth day here on Sunday for 91 and at the interval the tourists were 265 for six in their second innings -- a lead of 110 runs.
Denesh Ramdin was 23 not out and West Indies captain Darren Sammy unbeaten on four.
It seemed as if Chanderpaul was heading towards a 26th Test century when, he attempted to sweep the first ball of a new spell from off-spinner Graeme Swann and was given out lbw.
Chanderpaul, one of only 10 men in history to have scored 10,000 Test runs, immediately reviewed South African umpire Marais Erasmus's decision.
But replays indicated the ball would have hit the stumps and England had the wicket of the 37-year-old Guyana left-hander, one of the most obdurate batsmen in Test history.
With Chanderpaul having top-scored with 87 not out in West Indies's first innings 243, it meant he'd batted for 10 hours and 24 mins in this match, scoring 178 runs for once out -- a mammoth feat of concentration.
Together with Marlon Samuels he shared a fifth wicket stand of 157 that rescued the West Indies from the depths of 65 for four and a looming innings defeat in the first of this three-Test series.
The 31-year-old Samuels was closing in on what would have been only his third hundred in 38 Tests when, not long after England had taken the new ball, he played a tired-looking, flat-footed drive against Stuart Broad and edged straight to Swann at second slip.
A disappointed Samuels slowly trudged off, having faced 172 balls with 12 fours in three hours and 49 minutes of elegant resistance.
West Indies resumed Sunday on 120 for four, 35 runs behind, having lost three wickets with their score on 36 on Saturday.
Chanderpaul was 34 not out and Samuels 26 not out.
James Anderson and Broad, who'd taken a Test-best seven for 72 in the first innings, probed for an early breakthrough in overcast conditions but on what was still a typically good Lord's pitch.
But when Broad dropped short, Samuels pulled him past backward short-leg for four. And when the seamer repeated the dose next ball, Samuels commandingly pulled him in front of square for another boundary.
Samuels then reached his fifty in style by off-driving Anderson down the ground for four.
England captain Andrew Strauss switched to the spin of Swann in a bid to break the partnership.
However, Samuels cut Swann's first ball Sunday for a four that took the tourists into the lead and played a near carbon copy next ball.