Black Cat Cafe is located in the fifth ward of the Imperial Capital. Having lost their purpose after the war ended a few years prior, advanced mechanical dolls known as Automata have been restored and now work at the cafe wearing elegant kimonos. While they adjust to the peaceful world, events of the past continue to haunt the Automata, preventing them from letting go of the responsibility they once held. Among the Automata working at Black Cat Cafe is the recently restored Haizakura, who has lost her memories during a reset. Her identity and role in this unfamiliar world are a mystery to her, but one thing is certain—she loves to sing. With never-ending curiosity and beautiful songs to guide them, Haizakura and the Automata search for their new purpose together, supporting each other no matter how rigorous that endeavor might be.

In an era when Samurai ruled Japan… The Shinsengumi has been wiped out by an unknown attacker, leaving one survivor. Seven criminals are chosen as doubles for the Shinsengumi. To protect the security of Kyoto, a top-secret replacement operation is executed.

As another year begins at Yuigaoka Girls' High School, ushering in a fresh batch of students, the school idol club Liella! is excited to expand their membership. However, Liella! is extremely popular due to the astounding talent they have continuously displayed; thus, new students lack the courage to even consider approaching the club, fearing the rigorous training that might lie ahead. Amid her worries, club leader and co-founder Kanon Shibuya meets first-year student Kinako Sakurakouji and tells her about the world of school idols. This leaves Kinako in awe, but being fairly average herself, she feels she would not be capable of matching the spirited performances of the brilliant Liella! members. Nonetheless, Kinako receives encouragement to join the group and comes to share their dream of reaching for the stars once again in the grand Love Live! Competition.

The number of terrorist acts in Japan has never been lower, thanks to the efforts of a syndicate called Direct Attack (DA). The organization raises orphaned girls as killers to carry out assassinations under their "Lycoris" program. Takina Inoue is an exceptional Lycoris with a strong sense of purpose and a penchant for perfection. Unfortunately, a hostage situation tests her patience, and the resulting act of insubordination leads to her transfer out of DA. Not thrilled about losing the only place she belonged to, she reluctantly arrives at her new base of operations—LycoReco, a cafe in disguise. Takina's new partner, however, turns out to be quite different from what she imagined. Despite being the famed Lycoris prodigy, Chisato Nishikigi appears almost unconcerned with her duties. She drags Takina along on all kinds of odd jobs under the simple explanation of helping people in need. Takina is even more puzzled when Chisato takes down a group of armed assailants without killing any of them. Feeling like a fish out of water, Takina itches to get reinstated into DA—but Chisato is determined to prove to her that there is more to a life than just taking them.