Exandria Unlimited was created as a spin-off anthology series to explore new aspects of the Exandria setting and to help avoid burnout for the main Critical Role cast, especially Dungeon Master Matthew Mercer.

Aabria Iyengar, known for shows like Dimension 20 and Saving Throw, served as the first season's Dungeon Master, making her the first Critical Role show host other than Matthew Mercer.

Brennan Lee Mulligan was inspired to set Exandria Unlimited: Calamity in the Age of Arcanum after a 2021 dinner conversation with Mercer, during which Mercer mentioned the Age of Arcanum and the Calamity with a tone that convinced Mulligan it was a key unexplored part of his envisioned world.

For Exandria Unlimited: Divergence, Mulligan devised the concept of having players use 'level zero character' stat blocks, an idea further developed through a collaborative character creation session with the cast to capture a sense of helplessness for ordinary individuals.

Exandria Unlimited: Divergence was shot in a single week.

Zerxus Ilerez, a character played by Luis Carazo in Calamity, later appears in the third season of the animated series The Legend of Vox Machina, despite the character not existing until years after the original Vox Machina campaign concluded in canon.

Nydas Okiro, played by Lou Wilson in Calamity, subsequently appears in the first season of the animated adaptation The Mighty Nein.

In Critical Role's third campaign, Mercer dismissed the main cast at an ad break, including himself as Dungeon Master, and the episode resumed with Iyengar as Dungeon Master alongside the returning Kymal guest cast to wrap up the Crown Keepers storyline.