The electrodeposition from an acidic solution containing CU2+, Sn2+, and a cationic surfactant gave a negative differential resistance (NDR) and a current oscillation in a narrow potential region of about 20 mV lying slightly more negative than the onset potential for Sn-Cu alloy deposition. Scanning Auger microscopic inspection has indicated that alloy films deposited during the oscillation have a clear alternate multilayer structure composed of two alloy layers of different compositions. The multilayer had the period of thickness of 40-90 nm and was uniform over a macroscopically wide area of about 1 mm x 1 mm. Detailed investigations have revealed that the NDR arises from adsorption of a cationic surfactant (acting as an inhibitor for diffusion of metal ions) on the alloy surface, and the oscillation comes from coupling of the NDR with the ohmic drop in the electrolyte.