While on Earth in 2261, Kalomi met Spock, a Vulcan Starfleet officer. Kalomi immediately loved Spock and declared her feelings for him, but Spock could not return those emotions for her. Even after they parted company, Kalomi still carried feelings for Spock. (TOS episode: "This Side of Paradise", TOS novel: Inception)
In 2263, Kalomi joined Elias Sandoval's colonial expedition to Omicron Ceti III, and served as the groups senior biologist. When the expedition finally landing on Omicron Ceti III a year later, Kalomi discovered the pod plants and the contagious spores which they released into the atmosphere. While these spores protected the colonists from the deadly Berthold rays present in the atmosphere, they also gave the colonists a sense of contentment and perfect physical health.
Three years later, the USS Enterprise arrived in orbit of Omicron Ceti III to try and establish the loss of contact with the colony. Spock and Kalomi were quickly reunited, and she used one of the pod plants to infect Spock and break down his emotional controls so that he could love her in return. The couple spent many blissful hours together on the planet's surface, but the spores control over Spock was broken when Captain James T. Kirk was able to induce great anger in his first officer. Realizing that she had lost Spock once again, Kalomi broke down in tears. She later evacuated with the rest of the colonists to Starbase 27. (TOS episode: "This Side of Paradise"; TOS novel: The Fire and the Rose)