An ion-ion reaction route under solvothermal condition at relatively low temperatures was first put forward to the preparation of tetragonal Cu3SnS4 nanorods, on the basis of the strategy that 2D framework structure of Cu3SnS4 containing layers could provide orientation for the growth of quasi-1D nanomaterials, X-ray diffraction (XRD) pattern, transmission electronic microscope (TEM) images, electronic diffraction (ED) pattern, X-ray photoelectron spectra (XPS), energy-dispersive X-ray analysis (EDXA), Mossbauer spectrum, Raman spectrum, thermal analysis (DTA and TGA), ultraviolet and visible light (UV-vis) spectrum, and photoluminescence (PL) spectrum were used to characterize the products. On the basis of a series of supplementary experiments and the result of infrared absorption spectrum (IR), a reaction mechanism was proposed: ethanol as solvent and reductant and trace water/CH3CSNH2 as sulfur source and acid-making components could form 2D network through hydrogen bonds, which provided the orientation for the formation of a 2D framework structure; appropriate concentration of CH3CSNH2, warming speed, reaction constant temperatures (T-rc), and reaction time also played important roles.