Again, there are some repeats because there aren't enough villains in the League

Aries:
Magne

Taurus:
Mustard

Gemini:
Dabi

Cancer:
Spinner

Leo:
Kurogiri

Virgo:
All For One

Libra:
Shigaraki

Scorpio:
Mr. Compress

Saggitaroius:
Toga

Capricorn:
Magne

Aquarius:
Kurogiri

Pisces:
Dabi