In the process of surface treatment, steel wire brush can not only efficiently remove surface contaminants, such as deteriorated paint film and rust, but also increase the adhesive strength. However, the associated brush mechanics of material removal is still not clear. In order to reveal the brush mechanics of material removal, this paper assumed the tip of steel wire were ball–cone shaped, constructed contact force model, and calculated the brush grinding force under different process conditions based on finite element approach. The simulated results show that the brush grinding can be changed from plastic plowing to chip formation when the penetration depth is increased to 10 μm, then changed from chip formation to plastic plowing when the inclination angle is increased to 30°, respectively. The simulated value of brush force rises with the increasing penetration depth and inclination angle, which was consistent with the experimentally obtained values, and the relative errors are within 9%. The quantity of material removal increases with the ascending of penetration depth, and decreases with the ascending of inclination angle. This paper provides guidance to understand the mechanics of material removal, predict the brush grinding force, and contribute well to an automatic grinding control application.