SiO2 /Ni nanocomposite is directly prepared from the silica particle by a controllable method through electroless metallization, which is different from the sol-gel technique. Its fabrication procedure is as follows: first the formation of ligating monolayer by a silane agent coupling with silica, then, binding Pd catalyst with its ligating group, finally, nano-sized Ni deposition occurs on the template. The metallic Ni particles are uniformly deposited on the silica, and they have a net or chain-like structure, just as the silica particles do. The composite inherent coercivity (iHc), saturated magnetization (MS), and residual magnetization (Mr) are 16.5, 10.0 and 1.00 respectively in the as-plated Ni. The chain-like structure causes stronger static magnetization interactions between Ni particles, resulting in a magnetic crystalline anisotropy and the higher iHc value.