When war broke out between the Federation and the Klingon Empire in 2267, Captain James T. Kirk and Commander Spock met with Ayelborne and the Council to try to persuade them to side with the Federation and warn them of the imminent Klingon invasion. Ayelborne assured Captain Kirk that they had nothing to fear from the Klingons, but before a final decision could be made, the Klingon invasion force led by Kor arrived, and seized the planet.
Ayelborne quickly promised Kor that the Organians would not stand in their way and submit to their rules to avoid bloodshed. When Kirk and Spock began to initiate hostile action against the Klingon forces, Ayelborne and the rest of the Council took their true non-corporeal form and took action – Ayelborne simultaneously appeared on Organia, and the Federation and Klingon homeworlds, and imposed the Organian Peace Treaty, forcing an end to the war between the Federation and the Empire. (TOS episode: "Errand of Mercy")
When the Klingons launched a second war on the Federation in 2269, they stopped Ayelborne and the other Organians from interfering from placing a thought-shield around Organia. Captain Kirk and the USS Enterprise crew disabled the shield and contacted Ayelborne. As a result, Ayelborne removed the Klingons' space-travel abilities for a thousand years. (TOS novel: Spock Must Die!)
- Note: This particular story is severely incompatible with all subsequent canonical Star Trek productions.
While investigating Preserver obelisks on Loren V, Ayelborne immediately appeared to stop Kirk, Spock and Arex Na Eth from learning Preserver secrets. He said that the enforced peace had been squandered and that the Federation and Klingon Empire needed to earn peace for themselves. Ayelborne then appeared before the governments of the Federation and Klingon Empire, as he had done in 2267, and officially announced the end of Organian interference in their relations, on the condition that neither side was to pursue knowledge of the Preservers. (TOS - Year Four comic: "The Enterprise Experiment, Part 5")
Circa 2371, Ayelborne believed himself to be the last of the Organians, who had expanded their energies to enforce the peace. As his last act before departing this plane of existence, he hoped to initiate peace between the Federation and Romulans, much as he had started with the Federation and Klingons. To achieve this goal, he masqueraded as an unusual artifact, which was discovered by an expedition into the Gamma Quadrant sent out of Deep Space 9. He used his presence to bring together Starfleet ensign Jamie Samantha Kirk (a relation of James T. Kirk) and Romulan Ambassador Jannek (the son of Keras).
Unfortunately, the artifact also gained the attention of The Circle terrorist group, who believed it to be a Bajoran artifact called the Chalice, and stole it. Jannek, Kirk, and a rescue team from DS9 went to Bajor to retrieve it, and there Ayelborne revealed his true identity and his objectives, prompting Jannek to offer Ensign Kirk the role of liaison officer to the Federation. Satisfied that he had set the ball rolling, Ayelborne then departed this plane of existence. (DS9 comic: "Blood and Honor")