ZrO2-Al2O3 nanocomposite particles were synthesized by coating nano-ZrO2 particles on the surface of Al2O3 particles via the layer-by-layer (LBL) method. Polyacrylic acid (PAA) adsorption successfully modified the Al2O3 surface charge. Multilayer coating was successfully implemented, which was characterized by xi potential, particle size. X-ray diffraction patterns showed that the content of ZrO2 in the final powders could be well controlled by the LBL method. The powders coated with three layers of nano-ZrO2 particles, which contained about 12 wt% ZrO2, were compacted by dry press and cold isostatically pressed methods. After sintering the compact at 1450 degrees C for 2 h under atmosphere, a sintered body with a low pore microstructure was obtained. Scanning electron microscopy micrographs of the sintered body indicated that ZrO2 was well dispersed in the Al2O3 matrix.