The electrochemical CO₂ reduction reaction (CO₂RR) is an attractive method to produce renewable fuel and chemical feedstock using clean energy sources. Formate production represents one of the most economical target products from CO₂RR but is primarily produced using post‐transition metal catalysts that require comparatively high overpotentials. Here a composition of bimetallic Cu–Pd is formulated on 2D Ti₃C₂T_x (MXene) nanosheets that are lyophilized into a highly porous 3D aerogel, resulting in formate production much more efficient than post‐transition metals. Using a membrane electrode assembly (MEA), formate selectivities >90% are achieved with a current density of 150 mA cm⁻² resulting in the highest ever reported overall energy efficiency of 47% (cell potentials of −2.8 V), over 5 h of operation. A comparable Cu‐Pd aerogel achieves near‐unity CO production without the MXene templating. This simple strategy represents an important step toward the experimental demonstration of 3D‐MXenes‐based electrocatalysts for CO₂RR application and opens a new platform for the fabrication of macroscale aerogel MXene‐based electrocatalysts.

Noble metal aerogels as three-dimensional (3D) nanostructures with high surface area and large porosity are known to be exceptional materials that can be applied in the area of catalysis applications.