The high theoretical capacity of Bi2S3 shows high promise as a negative electrode material for energy storage devices. Herein, we investigate a facile, one-step chemical precipitation method using common organic solvents, such as acetone, ethanol, and isopropanol, for the synthesis of Bi2S3 nanostructures. The nanospherical Bi2S3 from acetone (Bi2S3-A) presents the most balanced electrochemical properties, exhibiting a high specific capacity of 181 mAh g−1 at 1 A g−1 and decent rate capability. Additionally, Bi2S3-A is used as a negative electrode in an aqueous hybrid system with an activated carbon positive electrode, demonstrating a capacitance of 86 F g−1, a specific energy of 7.6 Wh kg−1, and an initial capacity retention of 74% after 1000 cycles.