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The controllable preparation of noble metallic nanocrystals with a 3D architecture is of great interest for electrocatalysis applications due to their enhanced atomic utilization, facilitated mass transport, and other attractive properties. In this work, a facile, one-pot, and surfactant-free method of synthesizing heterophase sponge-like Pd (S-Pd) is developed. The prepared S-Pd has a four-fold higher peak current density and better durability than a commercial Pd/C catalyst for formic acid oxidation. It therefore has great potential as an anode catalyst for direct formic acid fuel cells.