In this paper, the prepared LaPO4/Al2O3 composite ceramics were ground by the surface grinding machine. The phase composition and morphology of the coated powders as well as the microstructure of grinding surface of the ceramics were characterized by X-ray diffraction (XRD), Transmission electron microscopy (TEM) and Scanning electron microscope (SEM), respectively. The results show that the coated powders have a distinct core-shell structure which has a great effect on material’s removal approaches. The main fracture mode is caused by intragranular fracture of layered LaPO4 rather than the weak interface. Besides, the primary grinding removal mechanism of LaPO4/Al2O3 composite ceramics mainly rise from cracks propagating along the interlayer of LaPO4.