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As a species they were warlike and did not believe in government, so they lived in a state of total anarchy where only the strong survived. They could only digest flesh that was either raw or still living, and could only survive three or four days without food. This meant that they did not adapt as well to captivity as other species like Humans, Bolians or Mizarians. (TNG episode: "Allegiance")
While attending Starfleet Academy, cadets Jean-Luc Picard and Cortin Zweller encountered Chalnoth mercenaries on the planet Yrskatdon while seeking medical attention for their classmate Marta Batanides. (SA comic: "Judgment")
While serving as captain of the USS Stargazer in 2354, Picard was dispatched to the Chalnoth homeworld of Chalna (known on Federation star-maps as Kaus Borealis V) in order to negotiate a dispute about a Federation research colony on the planet Ynathaia, which the Chalnoth claimed as their own. Picard defeated a Chalnoth champion in a trial by combat, through which Picard secured the safety of the colony until their research was done. (TNG comic: "Children of Chaos")
In 2366, a Chalnoth named Esoqq was kidnapped (along with Picard and several others) by a previously unknown (and unnamed) alien race that was studying the concept of leadership. (TNG episode: "Allegiance")
In 2370, while investigating the disappearance of the Federation vessel USS Aquitaine near the planet Beta Scoraata II, the USS Enterprise-D found both the Aquitaine and the Chalnoth vessel Blade seemingly abandoned. An away team from the Enterprise rescued the crews of the Aquitaine and the Blade from an indigenous creature that had encased both parties in cocoons, while Picard dealt with Chalnoth warships in orbit. After producing the rescued Chalnoth to the Chalnoth captain, Pathox, the Enterprise and the Aquitaine were allowed to leave the system unmolested. (TNG comics: "Children of Chaos", "Mother of Madness", "Brothers in Darkness")
In early 2377, a Chalnoth bounty hunter named Grauq unsuccessfully hunted the Cardassian woman Iliana Ghemor of the mirror universe on the planet Harkoum, but was killed during the pursuit. (DS9 novel: Warpath)