Highly efficient hydrogen generation from formic acid is a vital process in the clean energy and chemical industry fields. In this work, a universal and efficient surface‐amine‐implanting approach (SAIA) was proposed to fabricate highly active nanocatalysts with controllable nucleation and growth of small‐sized metal nanoparticles (NPs) and desired environments around the active sites. The highly dispersed ultrafine palladium NPs supported by the amine‐implanted porous carbon (Pd/APC) exhibited catalytic activity that was increased nearly threefold relative to that of the unmodified catalyst and showed high selectivity for the dehydrogenation of formic acid under mild conditions. Detailed investigations demonstrated that the amine species densely implanted on the pore surface of carbon by hydrothermal treatment with ammonium hydroxide played an important role in dispersing the metal NPs and in promoting the catalytic processes. The presented approach provides powerful entry into highly active catalysts to elicit enhanced catalytic performance for various catalytic reactions and to promote the dehydrogenation of formic acid for practical applications.