Burr-like Cus/9S5 microwires and Cu9S 5 microspheres can be synthesized by a two-step solvothermal method. Experiment results indicated that the CuS/Cu9S5 microwires (diameter of ca. 300 nm and length of several micrometers) and Cu 9S5 microspheres (diameter of ca. 800 nm) obtained by this method had uniform morphologies and large product. X-ray diffraction (XRD), high-resolution transmission electron microscopy (HR-TEM), and field-emission scanning electron microscopy (FE-SEM) experiments were carried out to characterize them. Fourier transform infrared (FT-IR) spectra and thermogravimetric analysis (TGA) experiments were carried out to study the components and thermal stabilization of the precursors. A possible formation mechanism and ultraviolet-visible (UV-vis) absorption spectra are also described inthis paper.