Design of cost-effective,yet highly active electrocatalysts for nitrogen reduction reaction (NRR) is of vital significance for sustainable electrochemical NH3 synthesis.Herein,we have demonstrated,from both computational and experimental perspectives,that FeTe2 can be an efficient and durable NRR catalyst.Theoretical computations unveil that FeTe2 possesses abundant surface-terminated and low-coordinate Fe sites that can activate the NRR with a low limiting potential (-0.84 V) and currently impede the competing hydrogen evolution reaction.As a proof-of-concept prototype,we synthesized FeTe2 nanoparticles supported on reduced graphene oxide (FeTe2/RGO),which exhibited a high NRR activity with the exceptional combination of NH3 yield (39.2 μg h-1 mg-1) and Faradaic efficiency (18.1%),thus demonstrating the feasibility of using FeTe2 and other earth-abundant metal tellurides for electrocatalytic N2 fixation.