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Willow Rosenberg and Tara MaclayHistorically significant as a groundbreaking LGBT relationship on television, Willow and Tara have instant chemistry from the moment they meet - in the Buffy Season 4 episode "Hush" - and are together for 2 years until Willow's dark magic leads to a break up. In a cruel twist, the two are finally together again for just 24 hours before Tara is shot and killed by bullets intended for Buffy.
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Spike & DrusillaDrusilla sired Spike, and the two were together for over 100 years until Dru realized Spike had fallen for Buffy.
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Darla and DrusillaDarla and Drusilla were known to be intimate with each other at least once (with The Immortal in the 1800s) but it's implied that there's far more of a history than just that.
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Buffy Summers and SpikeSpike and Buffy have a violent but passionate love/hate relationship that begins when Spike first crashes into town early in Season 2 on Buffy. In the series finale of the show, Spike dies for Buffy and Buffy finally tells him that he loves her - only to have him insist that she does not. Spike is later resurrected on Angel the Series, and his love for Buffy continues on.
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Faith Lehane and Buffy SummersFaith and Buffy... an interesting relationship to say the least. While they never actually get together, the sexual undertones to this pairing have been confirmed by enough writers as 100% intentional that "Fuffy" counts as canon. Let's not forget that those forehead kisses were originally written to be kisses on the lips.
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