Trigun

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Trigun is a 1990s Space Western manga-turned-anime. Set in the 32nd century on the hostile desert world of Gunsmoke, it revolves around two insurance agents, Meryl Stryfe and Milly Thompson, being sent by their boss to tracki down Gunsmoke's most infamous outlaw - Vash "The Stampede", "The Humanoid Typhoon", the Man With the $$66 Billion Bounty - and find out why he leaves such a swathe of destruction in his wake before their company goes bankrupt. Somehow, against all odds, they succeed... and discover Vash is a sweet-tempered goofball who is totally devoted to the ideal of pacifism; all the destruction is caused by the bounty hunters chasing after him.

...But, what about the destruction of the City of July, the crime that earned Vash his ridiculously high bounty?

Well, it turns out Vash has a brother; Knives. A brother who wants to complete the genocide of humanity he tried and failed at when he got them stuck on this inhospitable sand-clod in the first place. And he wants Vash to join him in wiping out humanity... even if this means breaking his mind and his spirit with massacres first...

This series is /tg/-relevant mainly because it's one of several popular late 80s-early 2000s anime to get licensed by Guardians of Order, either as setting splatbooks for Big Eyes, Small Mouth or fully marketed as "The Roleplaying Game" of their respective series.