Abstract: The composite of carbon nanotubes/graphene spheres-nano Ni (CNTs/GR-Ni) was synthesized by spray drying technology and heat treatment process. The adsorption property and catalytic performance were researched. The results showed that the composite of carbon nanotubes/graphene spheres loaded nano-Ni was successfully fabricated by spray drying technology and heat treatment process and Ni nanoparticles were distributed uniformly on the surface of carbon nanotubes/graphene microspheres. CNTs/GR-Ni had excellent adsorption property and magnetic separation property. Compared with the element Ni, CNTs/GR-Ni had the excellent catalytic performance and it made the temperature of high temperature decomposition of ammonium perchlorate decrease by 135℃.