Abstract: A unique hydrangea viburnum-like cobalt sulfide (HVCS) with multiple electrochemically active sites was successfully fabricated by a simple solvent thermal method. Polyaniline (PANI) was assembled onto the surface of HVCS through in situ polymerization and finally PANI were further carbonized to obtain hydrangea viburnum-like cobalt sulfide@nitrogen-rich carbon composite (HVCS@NC). Benefiting from the unique microstructure design and synergistic effect produced through the complementary properties of the two components, the fabricated HVCS@NC electrode demonstrates ideal electrochemical performance for supercapacitors through electrochemical analysis. The material exhibits an outstanding capacitive performance of 622 F·g⁻¹ at a current density of 1 A·g⁻¹ and the assembled asymmetric supercapacitor with HVCS@NC and active carbon (AC) as positive and negative electrodes, respectively, achieves a high specific energy of 19.9 W·h·kg⁻¹ at a specific power of 1912.3 W·kg⁻¹. All results show that high-performance supercapacitor electrode materials can be obtained by assembling conductive polymers on the surface of novel cobalt sulfide with special microscopic morphology and structure and then carbonizing. The plasticity and nitrogen-rich properties after carbonization of polyaniline have great advantages for improving the electrochemical performance of transition metal sulfide. This structural design strategy can be potentially extended to the improvement of electrochemical properties of other transition metal sulfide based electrode materials.