The development of cost-effective heterogeneous catalysts for the dehydrogenation of formic acid (FA) is the key challenge for the commercialization of FA as a hydrogen-storage medium. Herein, PdCoNi nanoparticles (NPs) with different element ratios supported on N-doped carbon nanosheets (N-CN) were designed, which exhibit excellent catalytic dehydrogenation performance for FA. Compared with PdCoNi NPs loaded on the carbon nanosheets (CN), the introduction of pyrrolic N to CN induces the formation of ultrafine, monodispersed and amorphous Pd0.6Co0.2Ni0.2 NPs with a size of 1.60 nm, which significantly increases the number of active sites and the instant contact between FA and catalysts. The as-prepared Pd0.6Co0.2Ni0.2/N-CN catalyst shows more than 99% conversion and 100% H-2 selectivity at room temperature, with a record-high initial turnover frequency (TOFinitial) of 1249.0 h(-1) among non-noble containing Pd-based catalysts, which demonstrates the high potential of Pd0.6Co0.2Ni0.2/N-CN as a practical catalyst for the hydrogen generation from FA. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.