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AbstractThe electrochemical carbon dioxide reduction reaction (CO2RR) provides a sustainable strategy to relieve global warming and achieve carbon neutrality. However, the practical application of CO2RR is still limited by the poor selectivity and low current density. Here, the surface molecular functionalization of unusual phase metal nanomaterials for high‐performance CO2RR under industry‐relevant current density is reported. It is observed that 5‐mercapto‐1‐methyltetrazole (MMT)‐modified 4H/face‐centered cubic (fcc) gold (Au) nanorods demonstrate greatly enhanced CO2RR performance than original oleylamine (OAm)‐capped 4H/fcc Au nanorods in both an H‐type cell and flow cell. Significantly, MMT‐modified 4H/fcc Au nanorods deliver an excellent carbon monoxide selectivity of 95.6% under the industry‐relevant current density of 200 mA cm−2. Density functional theory calculations reveal distinct electronic modulations by surface ligands, in which MMT improves while OAm suppresses the surface electroactivity of 4H/fcc Au nanorods. Furthermore, this method can be extended to various MMT derivatives and conventional fcc Au nanostructures in boosting CO2RR performance.