In this work, the anisotropic deformation and anisotropic mechanical properties of 4H silicon carbide (4H-SiC) single crystal wafers are proposed using nanoindentation. The C face of 4H-SiC wafer shows higher hardness and lower fracture toughness than those of the Si face. Because the deformation of 4H-SiC is assisted by the nucleation and slip of basal plane dislocations (BPDs), especially the slip of the Si-core partial dislocation (PD) of the BPDs, the nucleation and slip of the Si-core PD in the Si face of 4H-SiC is easier than those in the C face, which releases the nanoindentation-induced stress and results in the decrease of the hardness and increase of the fracture toughness of the Si face of 4H-SiC wafers. Due to the hexagonal lattice of 4H-SiC, the hardness along the 〈11 ̅00〉 direction of 4H-SiC is higher than that along the 〈112 ̅0〉 direction, but the fracture toughness along the 〈11 ̅00〉 direction is lower than that along the 〈112 ̅0〉 direction, as a result of the enhanced glide of dislocations along the most closely packed direction. The insights gained in this work are expected to shed light on the optimization of the mechanical processing of 4H-SiC wafers.