A series of cobalt-based catalysts supported on several acidic/basic oxides were prepared by the incipient wetness impregnation method and applied for the one-pot synthesis of isophorone diamine (IPDA) from hydroamination of isophorone nitrile (IPN). The effects of the supports and cobalt loading on the performance of the catalysts were investigated. The results showed that the Co/SiO2 catalyst with 20 wt % Co loading gave the highest conversion of IPN (90.9%) and yield of IPDA (70.4 mol %) among the supported cobalt catalysts used in this work, and it could be reused eight times without a significant decrease in the catalytic performance, which was much better than that from the commercial Raney Co. Meanwhile, the possible intermediates and reaction pathways during hydroamination of IPN were provided.