A facile microwave-biomolecular assistance method has been used to synthesize copper sulfide nanomaterials. In this process, the histidine as the directing and assembling agent plays an important role in the formation of the different hierarchical architectures. The morphologies and the sizes of the products can be tuned by adjusting the molar ratio of Cu2+/histidine and Cu2+/thiourea. The effect of other experiment parameters such as the reaction temperature, the power of microwave irradiation, and reaction time on the morphology and the size has been also discussed in detail. The possible reaction and growth mechanisms of the formation different hierarchical architectures are also discussed. In addition, the optical properties of these copper sulfides nanomaterials were investigated and the photocatalytic activity of different hierarchical architectures has been tested by the degradation of methyl orange (MO) under UV-light irradiation.