"Love Live! Superstar!!" centers on a group of high school girls who form an idol group to save their school from closure. The story is set at Yuigaoka Girls' High School, a newly established institution in the Odaiba area of Tokyo. The protagonist, Kanon Shibuya, is a shy and reserved first-year student who loves singing but struggles with stage fright. Her life changes when she encounters a poster promoting the school's idol club, sparking her interest in joining.

Kanon is soon joined by four other students: Keke Tang, a transfer student from Shanghai who is passionate about idols; Chisato Arashi, a childhood friend of Kanon who is initially hesitant about the idea of becoming an idol; Sumire Heanna, a confident and ambitious girl with a flair for performance; and Ren Hazuki, a quiet and mysterious student with a natural talent for music. Together, they form the idol group Liella! and begin their journey to compete in the Love Live! competition, a prestigious idol event that could bring recognition and save their school.

The narrative explores the challenges the group faces as they balance their studies, personal struggles, and the demands of being idols. Each character brings unique strengths and vulnerabilities to the group, and their interactions highlight themes of friendship, perseverance, and self-discovery. The series delves into their growth as individuals and as a team, emphasizing the importance of collaboration and mutual support.

As Liella! gains popularity, they encounter rival idol groups and navigate the competitive world of school idols. The story also touches on the pressures of fame and the sacrifices required to pursue their dreams. Through their performances and experiences, the members of Liella! inspire each other and their audience, showcasing the transformative power of music and shared goals.

The series maintains a balance between lighthearted moments and emotional depth, with a focus on character development and the bonds formed within the group. The narrative progresses through their journey to the Love Live! competition, culminating in a climactic performance that tests their resolve and unity. "Love Live! Superstar!!" is a story of ambition, camaraderie, and the pursuit of dreams, set against the vibrant backdrop of the school idol phenomenon.