After topping the podium in Beijing and London, the Netherlands were hot favourites going into the Rio Games.
Despite winning every game to finish top of their group, however, the top-ranked Dutch team only scraped into the final after beating ninth-ranked Germany 4-3 in a shootout following a 1-1 draw.
Britain also finished the group stages with a perfect record and were gunning for gold in their first Olympic final having won bronze four years ago in London. Germany beat New Zealand 2-1 to take the bronze medal.
"We've done it," British midfielder Nicola White told reporters, brandishing her medal with a grin plastered across her face. "We've trained our arses off for so long, this is what we've dreamed of and now we've got it.
"We've now gone unbeaten through an Olympic tournament, which is unreal," she added. "We are just over the moon."
That the near sell-out crowd at the Olympic Hockey Centre, a venue which has struggled to fill seats during the Rio Games, were in for a show was clear from the pushback.
A boisterous British tackle and ensuing penalty flick gave Dutch captain Maartje Paumen an early chance to score, but her shot was batted aside by British keeper Maddie Hinch.
'SHAME IT'S SILVER'
Britain's Lily Owsley claimed the first score of the night, emerging victorious from a mad scramble in front of the Dutch goal to put her side 1-0 ahead.
A Dutch equaliser came courtesy of forward Kitty van Male who broke away for a one-on-one with the British keeper, skilfully drawing her aside and putting the ball into the top of the net with an audacious reverse stick sweep.
The Netherlands' second goal promptly followed with Paumen scoring off the last of three penalty corners in the space of four minutes. Seconds later, Britain's Crista Cullen picked up a cross in the opposition circle to level the scores at 2-2 going into the break.
The goals kept coming in the second half. Both teams netted one each after a series of penalty corners, leaving the score deadlocked at 3-3 on the final whistle and forcing a shootout to decide the match.
Of the 10 goals available, only two were scored. Britain's Helen Richardson-Walsh and Hollie Webb found the back of net to secure victory and their team's first Olympic gold medals.
"We played very well during the game. I think we played way better than them," said the Netherlands' Eva de Goede. "But shootouts are fifty-fifty. They won, we lost, it's tough."
"Shame it's silver," she added, gesturing to the medal which will join the two gold ones she already has at home. "We were really going for a third gold. But it didn't work out."
(Editing by Ed Osmond and Meredith Mazzilli)
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