Silicon nitride ceramic composites were densified by spark plasma sintering with different-sized Mo particles. In-situ synthesis of Mo-Si compound can accelerate the nucleation of β-Si3N4 grain, and the number of β-Si3N4 grain nucleation increases with decrease of Mo particle size during spark plasma sintering. The effect of Mo particle size on the grain growth of β-Si3N4 is significant, while that for the phase composition of Si3N4 samples is negligible. Si3N4 ceramic composites with 6 wt% nano-sized Mo addition are shown to have the highest bending strength (922.56 MPa) and fracture toughness (8.94 MPa m0.5), which is attributed primarily to more elongated β-Si3N4 grains obtained by more β-Si3N4 grain nucleation.