Calcined fly ash (CFA) was first obtained by calcining fly ash (FA) at 815 °C for two hours. Then, composite powders of CFA coated with zinc oxide nanoparticles (ZnO/CFA, ZCFA) were prepared by heterogeneous nucleation method. The samples were characterized by X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, Scanning electronic microscopy (SEM), Whiteness, and Brunauer-Emmett-Teller specific surface area (BET). Effects of pH value, reaction temperature and time, coating amount, solid-to-liquid ratio, the coating agent concentrations, and dropping speed on the whiteness of ZCFA powders were studied. It was shown that after coated with ZnO particles, the whiteness of CFA was increased from 27.0 to 62.6%, and the specific surface area was increased from 5.80 to 14.61 m2/g. Needle ZnO with the average grain size of 46 nm was deposited on the surface of CFA. Si–O–Zn–OH bonds were formed.