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 blood-shed. 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. Thankfully, Captain Kirk and the USS Enterprise crew were able to break down the shield and contact Ayelborne. As a result Ayelborne removed the Klingons space travel abilities. (TOS novel: Spock Must Die!)
Circa 2371 Ayleborne 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 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 got the attention of The Circle, 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 Kirk the role of being his liaison officer to the Federation. Satisfied he had set the ball rolling Ayleborne then departed this plane of existence. (DS9 comic: "Blood and Honor")