AbstractHydrogen (H2) is recognized as a clean energy carrier with great potential for the future energy systems. Given the existing challenges in direct H2 storage and delivery, the current option for utilizing hydrogen energy is to produce hydrogen from its storage carriers on‐site, and the development of a highly active, highly selective, and highly stable catalyst for H2 production is an important part of this. Herein, PdAg alloy was deposited on mesoporous carbon nitride (mpg‐C3N4) as a catalyst for the dehydrogenation of the formic acid (FA). The synergistic effect of Pd and Ag metals for catalysis was explored. The role of the supports on the catalytic performance was also demonstrated by depositing PdAg alloy on several carriers of Silica@Resorcinol‐Formaldehyde Spheres, Carbon Flower Particles and SBA‐15. Pd1Ag1/2/mpg‐C3N4 showed a considerable activity during FA dehydrogenation with a turnover frequency (TOF) value of 887 h−1 at 333 K, demonstrating that carbon nitride as a carrier has a significant enhancement on the catalytic hydrogen production from formic acid.