Ammonia is a potential fuel for producing and storing hydrogen, but its usage is constrained by the high cost of the noble metal catalysts to decompose NH3. Utilizing non-precious catalysts to decompose ammonia increases its potential for hydrogen production. In this study, carborundum (SiC)-supported cobalt catalysts were prepared by impregnating Co3O4 nanoparticles (NPs) on SiC support. The catalysts were characterized by high-resolution transmission electron microscope, X-ray photoelectron spectroscopy, temperature programmed reduction, etc. The results show that the large specific surface area of SiC can introduce highly distributed Co3O4 NPs onto the surface. The amount of Co in the catalysts has a significant effect on the catalyst structure, particle size and catalytic performances. Due to the interaction of cobalt species with SiC, the 25Co/SiC catalyst provided the optimal ammonia conversion of 73.2% with a space velocity of 30,000 mL gcat −1 h− 1 at 550 °C, corresponding to the hydrogen production rate of 24.6 mmol H2 gcat −1 min− 1. This research presents an opportunity to develop highly active and cost-effective catalysts for hydrogen production via NH3 decomposition.