Polythiocyanogen, (SCN) x , is a promising lithium-ion battery electrode material due to its high theoretical capacity (462mAhg−1), safe operation, inexpensive raw materials, and a simple and less energy-intensive manufacturing process. The (SCN) x was prepared from the solution of trithiocyanate (SCN)3 − in methylene dichloride (MDC), which was prepared by electrochemical oxidation of ammonium thiocyanate (NH4SCN) in a two-phase electrolysis medium of 1.0M NH4SCN in 0.50M H2SO4 +MDC. The (SCN)3 − underwent auto catalytic polymerization to (SCN) x during MDC removal. Battery electrodes with (SCN) x as the active material were prepared, and tested in Swagelok cells using lithium foil as the counter and reference electrode. The cells delivered capacities in the range of 200–275mAhg−1 at the discharge–charge rate of 0.2C. The cells were tested up to 20 cycles and showed repeatable performance with a coulombic efficiency of 97% at the 20th cycle. The results presented here indicate that (SCN) x is a promising lithium-ion battery electrode-material candidate for further studies.