AbstractIn this work, highly efficient carbon‐supported Pd‐based catalysts for formic acid dehydrogenation were synthesized by a straightforward wet impregnation‐reduction method. The carbon support was obtained from a biomass residue (almond shell) prepared via H3PO4‐assisted hydrothermal carbonization (HTC) and thermal activation. This carbon support was doped with nitrogen groups to study the effect on the electronic properties and catalytic performance of the catalysts. Investigating the formation of PdAg alloys with varying Pd : Ag molar ratios resulted in catalysts exhibiting enhanced catalytic activity compared to monometallic Pd counterparts. Notably, the Pd1Ag0.5/NAS catalyst displayed outstanding catalytic performance, achieving an initial TOF of 1716 h−1 (calculated in the first 3 minutes of reaction and expressed per mole of Pd) and maintaining substantial activity over 6 consecutive reaction cycles. This work elucidates the successful synthesis of effective catalysts, emphasizing the influence of nitrogen doping and PdAg alloy composition on catalytic behavior and stability.