As a typical brittle crystal material, single crystal silicon has high hardness and brittleness, which makes the machined surface prone to microscopic cracks and other subsurface damage. In addition, the anisotropic crystal structure may cause large differences in the material removal behavior along different crystal orientations. To solve these problems, researchers have proposed the methods of machining along the easy-to-cut direction and inducing external energy fields assisted machining, but there remain problems like cracks and surface thermal damage. In this study, we propose to modulate the deformation process of single crystal silicon by atmospheric pressure cold plasma and elucidate the influence of plasma on the material removal behavior based on diamond grit scratching experiments along different directions. The results show that before plasma treatment, the toughness along <110> direction is higher than that along <100> direction, and plasma has significant improvement effects on the plastic deformability in both directions. The critical load for plastic-brittle transition along <110> direction can be increased from 76.2 mN to 107.1 mN, and from 69.6 mN to 109.8 mN along <100> direction. The plasticity regulation mechanism is that the interaction of multiple shear bands dissipates the energy of crack propagation and inhibits the premature generation of cracks. Compared with the conventional scratching along <110> direction, the material removal rate of plasma-assisted scratching under normal loads of 20 mN, 40 mN and 80 mN can be increased by 30.2%, 24.2% and 21.9%, respectively; while that along <100> direction can also be increased by 33.7% and 19.5% under 20 mN and 40 mN, respectively. This study may provide a novel approach for realizing high-quality and efficient processing of hard and brittle materials.