Flower-like Bi2S3/MoS2 nanohybrids with high-quality heterostructures and three-dimensional asile exhibit a remarkable electrochemical performance for supercapacitors. Display omitted •Three-dimensional (3 D) flower-like Bi2S3/MoS2 nanohybrid was synthesized by facile one-pot hydrothermal method.•MoS2 nanosheet is tightly attached to the surface of the Bi2S3 nanorod to form superior heteroinface.•Flower-like Bi2S3/MoS2 nanohybrid was assembled from Bi2S3 nanorod /MoS2 nanosheet heterostructures.•The as-prepared flower-like Bi2S3/MoS2 nanohybrid exhibits excellent electrochemical performance.•The results bring a new strategy to design advanced electrode materials for high-performance supercapacitors. Three-dimensional (3D) flower-like Bi2S3/MoS2 nanohybrid is synthesized using a facile one-pot hydrothermal method. In the nanohybrid, MoS2 nanosheet is tightly attached to the surface of the Bi2S3 nanorod to form a superior heterointerface, facilitating the electron transfer. Three-dimensional nanoarchitecture gives rise to large spaces and voids, fastening the ion diffuse. With the unique structural features of high-quality heterostructures and 3D aisles, the as-prepared flower-like Bi2S3/MoS2 nanohybrid exhibit excellent electrochemical performance with a high specific capacitance of 3040Fg−1, a remarkable rate capability (1258Fg−1 at a current density of 30Ag−1), and an outstanding cycle stability (92.65% capacitance retention after 5000 cycles at 10Ag−1). These promising results bring a new strategy to design advanced electrode materials for high-performance supercapacitors.