Scorpio: Levi and Eren (Attack on Titan)

Virgo: Gray and Natsu (Fairy Tail)

Gemini: Yukio and Rin Okumura (Blue Exorcist)

Cancer: Annie Leonhardt and Mikasa Ackerman (Attack on Titan)

Aquarius: Jean Kirschtein and Eren Jaeger (Attack on Titan)

(These signs and characters are the only ones I assign them as "Cat and Mouse" :') XD )