The cult was unofficially formed when Jaha and eleven other Sky People ventured into the Dead Zone to search for the City of Light. Some members of the group left to return to Camp Jaha, and some died along the way. Only Jaha and Murphy made it to the island, where Jaha abandoned Murphy at the lighthouse bunker. Murphy was locked in the lighthouse for 86 days, and when he was let free, Jaha had joined A.L.I.E., officially starting the cult.
The group was formed by A.L.I.E., who claimed to offer people a better existence in the City of Light, a virtual reality utopian city. The promise of eternal life in this beautiful place free of pain, suffering, and loss attracted many adherents among the outcasts of society, who risked their lives traveling the Dead Zone in search of it.
In the advent of a second apocalypse, A.L.I.E. gained the means to leave the island and began a forceful recruitment of followers. Her goal was to have all humans swallow the Key to the City of Light, a neural chip. This would enable her to control them, link their minds linked to one another, and allow them to access the City of Light. A.L.I.E. claimed she was doing this to save humanity.
During the conflict against A.L.I.E., A.L.I.E. controlled the minds of a large amount of people within the Arkadia-Polis area in Eastern North America. A.L.I.E.'s associates convinced hundreds of Sky People and thousands of Grounders from the Coalition to swallow the chip. When Clarke terminated A.L.I.E., she freed everyone from A.L.I.E.'s control, thus dissolving the cult.
During their campaign, A.L.I.E. and her followers took over a large amount of land otherwise belonging to non-brainwashed peoples. The original location of the cult was the island near the Dead Zone on which A.L.I.E. resided for 97 years until Thelonious Jaha discovered her and helped her relocate. The first place to be taken over by the followers of A.L.I.E. was the Skaikru settlement of Arkadia, thanks to the help of Doctor and Former Chancellor, Abigail Griffin, who allowed the sharing of the chips to almost every resident within Arkadia's walls.
A.L.I.E.'s new army of chipped Arkadians soon made their way to the Coalition capital of Polis, where they recruited thousands of Grounders to their cause and those who resisted the takeover were either imprisoned or crucified.
In Season Four, it is revealed that A.L.I.E. also gained influence and territory in the Trishanakru clan, with Ilian torturing one of his loved ones so they would take the chip. This means that A.L.I.E. and her cult took control of the clans Skaikru, Trikru, Floukru, Trishanakru, Azgeda and possibly others.