In this paper, we report on the microwave absorbing properties of the Ni/SiO2 core/shell soft magnetic material which was synthesized by the tetraethyl orthosilicate (TEOS) hydrolysis method. The SEM patterns were shown that the particles of Ni/SiO2 were more dispersed and homogeneous. Microwave absorbing properties were measured in the range of 0.1–18 GHz. A reflection loss (RL) exceeding −20 dB in the frequency range of 2.6–8.9 GHz was achieved for an absorber thickness of 2.0–5.6 mm, and an optimal RL of −49.5 dB was obtained at 4.4 GHz for the thickness of 3.5 mm. The good microwave absorption properties resulted from a proper impedance match as a consequence of the insulator SiO2 around Ni particles.