In order to investigate the failure process of brittle rock under triaxial compression through both experimental and numerical approaches, the particle simulation method was used in numerical simulations and the simulated results were compared with those of the experiment. The numerical simulation results, such as fracture propagation, microcrack distribution, stress-strain response, and damage patterns, were discussed in detail. The simulated results under various confining pressures (0–60 MPa) are in good agreement with the experimental results. The simulated results reveal that rock failure is caused by axial splitting under uniaxial compression. As the confining pressure increases, rock failure occurs in a few localized shear planes and the rock mechanical behavior is changed from brittle to ductile. Consequently, the peak failure strength, microcrack numbers, and the shear plane angle increase, but the ratio of tensile to shear microcracks decreases. The damage formation during the compression simulations indicates that the particle simulation method can produce similar behaviors as those observed through laboratory compression tests.