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The electrochemical reduction of CO₂ into renewable chemical products such as formic acid is an important and challenging goal. Traditional Pd catalysts suffer from CO poisoning, which leads to current density decay and short operating lifetimes. Here we explored the ability to control Pd nanoparticle surface morphology to amplify catalytic activity and increase stability in the electroreduction of CO₂ to formate. Through computational studies we have elucidated trends in intermediate binding which govern the selectivity and catalytic activity. We then rationally synthesized Pd nanoparticles having an abundance of high-index surfaces to maximize electrocatalytic performance. This catalyst displays a record current density of 22 mA/cm² at a low overpotential of −0.2 V with a Faradaic efficiency of 97%, outperforming all previous Pd catalysts in formate electrosynthesis. The findings presented in this work provide …