mo_lave,
hal_5700X, 
Maria+Holic Alive OP 1 Mousou Senshi Miyamae Kanako by Sugita Tomokazu
starman2112, 
Land of the Lustrous’ opening, Kyoumen no Nami, is my #1 most listened to song on Youtube Music two years in a row, so probably that.
Aside from that, some top picks are (in order of best to not as best)
Akudama Drive (mainly for the visuals)
Noir (also mainly for the visuals)
HipsterTenZero, (edited ) 
Steveanonymous, 
Ok I got more
Komi can’t communicate
m.youtube.com/watch?v=xHlx3rx5Bew
Gundam iron blooded orphans
m.youtube.com/watch?v=82HM0z6qd20
Black lagoon
emergencyfood,
- Inner Universe from GitS: SAC - if cyberpunk had a theme song, it would be this.
- No Separation from Heaven Official’s Blessing - a warm, slowly building love song with a hint of loss and longing.
- A Cruel Angel’s Thesis from NGE - an energetic, action-y song with darker undertones.
Veritrax, Evangelion - The Cruel Angel’s Thesis
raven369, Hero’s Come Back from Naruto Shippuden
Honorable mentions:
- SAO Crossing Fields
- Cowboy Bebop Tank
- Gurren Lagann Sorairo Days
nave,
Steveanonymous, m.youtube.com/watch?v=vIhQ9zya2-g
Gundam the witch from mercury
Any jojo op but especially great days
m.youtube.com/watch?v=mU3vgXUKeFM
And this one
AlfredEinstein,
eddanja, The one that’s always stuck with me is Blood+ third opening to the song of Colors of the Heart by UVERworld.
asymmetric, ClariS - Irony - OreImo season 1 OP
It’s so gahdamn catchy
NeryK, 
I thought my answer would be Ghost in the Shell Stand Alone Complex, because the theme song is so good. However I just rewatched it, and it’s full-on early 2000’s bad 3DCG.
My actual favorite overall has to be One Punch Man then.
Mint_Raccoon, 
I'd have to pick Butter-fly from Digimon Adventure.
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