The invention discloses a method for preparing a copper-zinc-tin-sulfur film material by a two-electrode system. The method comprises the following steps: (1) preparation of electrolytes: two electrolytes, i.e., a copper-tin mixed electrolyte and a zinc plating solution, are respectively prepared; (2) electrochemical deposition of a metal prefabricated layer: firstly, copper and tin metal layers are co-deposited by the two-electrode system; and then, a zinc metal layer is deposited to obtain a copper-zinc-tin metal prefabricated layer; (3) soft annealing and vulcanization of the metal fabricated layer: the copper-zinc-tin metal prefabricated layer is alloyed at low temperature under the nitrogen protection, and is vulcanized at high temperature under the sulfur atmosphere to prepare a copper-zinc-tin-sulfur film; and (4) cleaning of the surface of the copper-zinc-tin-sulfur film: the copper-zinc-tin-sulfur film is dipped in an organic solvent, is ultrasonically cleaned by de-ionized water, and is dried by nitrogen. Compared with a traditional three-electrode system partial deposition method, a two-electrode system copper-tin codeposition method has such advantages as convenience for operation and control, simple equipment and cost saving under the precondition of not reducing the quality of the copper-zinc-tin-sulfur film.