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I'll break my favorites into sections.
Bleach: Nearly all of them. But my top 5 favorites are
Ichigo in 2nd bankai form, which is my favorite character design.
Kenpachi with his wild hair and scars comes 2nd.
Urahara is so chill with his hat and hairstyle
Mayuri is just plain crazy with his facepaint and expressions
Unohana gives the gentle appearance till you make her angry lol.
Naruto: Minato's design just screams badass ninja.
Kakashi: Probably my most favorite character design from Kishi.
Jiraiya: His long hair is pretty awesome.
Itachi: Again another great character design.
Hinata: She always appears in the background as a serene individual. Her face has a nice structure too.
One Piece: To be honest I don't like Oda's designs all that much even if his characters are great.
Zoro: My favorite design from Oda.
Law: Another great design by Oda, especially the tattoos.
Reborn!: Mukuro: His pineapple hair makes for a great design.
Tsuna: His design fits his no good Tsuna personality, at least until he goes hyper mode.
Fairy Tail: Natsu: Looks like Haru who was well designed by Mashima before. Plus his hair is one of my favorite features about him.
Lucy: Those boobs were designed with her in mind lol.
Erza: I really like Erza's design and her different armors.
Astro Boy: Astro: Osamu designed Astro perfectly for his manga with his face and hair.
So many more that this post will get too long. I like designs from Ruronin Kenshin, Ultimate Muscle, Gintama, DBZ, YYH, HXH, R+V,
Sekirei, and many others I can't think of right now.
I like the contrast between Kogami and Maksihima's character designs from Psycho-Pass. Kogami's appearance is that of any average Japanese male with black hair and dark eyes. He primarily wears a formal dark suit and looks chic in the process. Makshima on the other hand does not look in anyway Japanese despite his name: he has white hair and amber eyes. His form of attire is casual and although he does wear clothes with some colour, it's still light in shade.
-D from Vampire Hunter D (Bloodlust version is the coolest looking)
-Shinkoyo from Hoshin Engi
-Yuko from XXXholic
-Holo from Spice and Wolf
I love Tower of God for its unique character designs so it's so hard to pick a favourite out of the bunch because they're all so neat!
If I had to choose, it would be Mule Love. Despite the countless number of non-human characters in the series, he looks the most out there. I love how he can put up a good fight despite his cute appearance.
Yes about ToG characters. I think Rachel is just such a great character. Completely and malevolently human! In fact, compared to Koon, Androssi, Hwa Ryun and Rak, Baam is somehow too simple and uninteresting.
I love Noblesse for its unique character design. Rai's and Frankenstein's design is cool.