As a novel type of green energy storage device, supercapacitors exhibit several orders of magnitude higher capacities than the traditional dielectric capacitors and significantly higher power density than the traditional secondary batteries. Supercapacitors have been widely applied in energy storage fields. Electrode materials, as pivotal components of supercapacitors, play an important role in electrochemical performance. Molybdenum-based materials have attracted widespread attention for their high theoretical capacitance, abundant resources, and facile synthesis tactics. Therefore, it is necessary to systematically summarize the application of Mo-based electrode materials in high-performance supercapacitors and unveil their developmental direction and trends. In this paper, we provide a review of binary Mo-based materials, ternary Mo-based materials, nanocomposites of Mo-based materials, and Mo-based MOFs and derivative materials. In addition, we further point out the key issues on the development of Mo-based materials in supercapacitors. This review may inspire more insightful works and enlighten other electrochemical areas concerning Mo-based materials.