5 Zodiac Signs That Are Libra Soulmates Libra heart most suitable zodiac signs are gemini, water bearer, and aries. When it comes to matters of the heart, Libra seeks harmony and compatibility above all else. Gemini can provide excitement and playfulness to the connection, while Aquarius shares Libra's appreciation for wisdom and originality. Aries, known for their intensity, can ignite a spark in Libra's soul. Libra and these signs create a well-rounded and rewarding partnership.