Unique MoS2-SnS2 heterogeneous nanoplates have successfully in-situ grown on poly(3-(1-vinylimidazolium-3-yl)propane-1-sulfonate) functionalized polypyrrole/ graphene oxide (PVIPS/PPy/GO). PVIPS can attract heptamolybdate ion (Mo7O246−) and Sn4+ as the precursors by the ion-exchange, resulting in the simultaneous growth of 1T’-MoS2 and the berndtite-2T-type hexagonal SnS2 by the interfacial induced effect of PVIPS. The obtained MoS2-SnS2/ PVIPS/PPy/GO can serve as electrocatalysts, exhibiting good NRR performance by the synergistic effect. The semi-conducting SnS2 would limit the surface electron accessibility for suppressing HER process of 1T’-MoS2, while metallic 1T’-MoS2 might efficiently improve the NRR electroactivity of SnS2 by the creation of Mo-Sn-Sn trimer catalytic sites. Otherwise, the irreversible crystal phase transition has taken place during the NRR process. Partial 1T’-MoS2 and SnS2 have electrochemically reacted with N2, and irreversibly converted into Mo2N and SnxNz due to the formation of Mo−N and Sn−N bonding, meanwhile, partial SnS2 has been irreversibly evolved into SnS due to the reduction by the power source in the electrochemical system. It would put forward a new design idea for optimizing the preparation method and electrocatalytic activity of transition metal dichalcogenides.