Bismuth nanosheets were recently shown to be excellent catalysts for the electrocatalytic nitrogen reduction reaction (NRR) to ammonia, and in addition, bismuth telluride iodide (BiTeI) has been labeled as a promising two-dimensional nanomaterial for energy applications, but it has been theoretically and experimentally investigated almost exclusively in its bulk state. Herein, we report for the first time the successful electrochemical exfoliation of BiTeI in DMF down to nanosheets of an average thickness of 10−20 nm without altering its hexagonal structure. The exfoliated nanosheets were evaluated for NRR, and they produced 1.04 ± 0.05 μg h −1 cm −2 of ammonia with a Faradaic efficiency of 1.67 ± 0.10% at −0.5 V vs Ag/AgCl in 0.1 M KOH.