Bi2S3 flowerlike patterns with well-aligned nanorods were synthesized using a facile solution-phase biomolecule-assisted approach in the presence of L-cysteine (an ordinary and cheap amino acid), which turned out to serve as both the S source and the directing molecule in the formation of bismuth sulfide nanostructures. Emphatically, no nauseous scent (H2S) appeared in our experiments, which could not be avoided in other previous reports. The morphology, structure, and phase composition of the as-prepared Bi2S3 products were characterized using various techniques (scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, selected area electron diffraction, and high-resolution transmission electron microscopy). The formation mechanism for the bismuth sulfide flowerlike assemblies with well-arranged nanorods was also discussed. In addition, other Bi2S3 homogeneous nanostructures (e.g., networklike nanoflakes, nanorod-based bundles, and nanoflakes) were obtained through varying the experimental parameters. Interestingly, we have found that these synthesized bismuth sulfide nanostructures using the biomoleucle-assisted approach could electrochemically charge and discharge with the capacity of 142 (mA h)/g (corresponding to 0.51 wt % hydrogen in single-walled carbon nanotubes) under normal atmosphere at room temperature. A novel two-plateau phenomenon was observed in the synthesized Bi2S3 nanostructures, suggesting that there were two independent steps in the charging process. It has been demonstrated that the bismuth sulfide's morphology and the constant charge-discharge current density had a noticeable influence on their capacity of electrochemical hydrogen storage. These differences in hydrogen storage capacity are likely due to the size and density of space/pores as well as the morphology of different Bi2S3 nanostructures. The novel Bi2S3 nanomaterials may find potential applications in hydrogen storage, high-energy batteries, luminescence, optoelectronic and catalytic fields, as well as in the studies of structure-property relationships. This facile, environmentally benign, and solution-phase biomolecule-assisted method can be potentially extended to the preparation of other metal chalcogenides including FeS, CuS, NiS, PbS, MnS, and CoS nanostructures.