AbstractGenerative adversarial networks (GANs), as a powerful tool for inverse materials discovery, are being increasingly applied in various fields of materials science. This review provides systematic investigations on the applications of GANs from a group of different aspects. The basic principles of GANs are first introduced; then a detailed review of GANs‐based studies regarding distinct scenarios across composition design, processing optimization, crystal structure search, microstructure characterization and defect detection is presented. At the end, several challenges and possible solutions are discussed and outlined. This overview highlights the efficacy of GANs in materials science, and may stimulate the further use of GANs for more intriguing achievements.