A coupled FEM-SPH numerical model is established to investigate the erosion behaviors of float glass subjected to angular particle impacts. The accuracy of the model is validated by comparing with measured data onto float glass erosion experiments. The model is then used to simulate single rhomboid particle impact on float glass surfaces under various conditions including impact velocity (20~110 m/s), impact angle (60~90 deg) and initial orientation angle (−10~50 deg). The results show: (1) similar to ductile material, the critical orientation angle marking the maximum kinetic energy loss is also observed for brittle material like float glass. Under the critical impact condition, the kinetic energy loss of rhomboid particle is up to 98.69% and 94.82% during vertical and incline impact respectively; (2) The formation and propagation of radial cracks and lateral cracks are determined by the combined effects of impact angle and orientation angle, and the brittle crater formed by the backward impact is wider and shallower than that of forward impact; (3) The behaviors of brittle splashing (i.e., fragments and chips) are successfully reproduced by the model, and the particle rotation behaviors after the impact significantly influences the direction of splashing stream which is less influenced by the impact angle; (4) The impact velocity determines the extent of material damages, and has little influence on the rotation behaviors of particle. Under the condition of constant kinetic energy, the size of particle (1.0~5.0 mm) has little effect on the erosion mechanisms in terms of crater depth, crater profile, splashing flow pattern and crack propagation.