 If you liked
Darker than Black: Kuro no Keiyakusha
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 ...then you might like
Baccano!
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Darker than Black follows a more episodic structure, but both of them have memorable soundtracks filled with jazz.
Has a wide cast of very contrasting characters, comic relief, and some good bloody action scenes.
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Recommended by shannontheme
Despite the fact that plot wise these two shows aren't very similar, they still resemble one another. Both shows feature adults, rather than children or teenagers. Hei also reminds me a bit of Firo, in the sense that they can both keep their calm and both are skillful at their speciality. There's also a certain amount of supernatural in both series and both are aimed at older audiences.
Both have good supernatural action (Darker than Black has more of this though). Similar moods, interesting characters. Both go back and forth between comical characters and serious moments. Darker than Black has more of a global story, Bacanno! is very focused on a small group.
Darker Than Black is obviously longer than Baccano!, but aside from that they have in common:
—The style of art;
—A similar tone of violence;
—There are mysteries to be solved by the viewer;
—More than one character to root for.
There's even one character in particular that is pretty much the same as in Baccano!, but you'll have to find out by yourself.
That said, I hope you give one of them a try ;D