The possibility of surface modification of thin polycrystalline aluminum nitride films by bombardment with argon cluster ion beam is investigated. The processing was carried out with high- (105 eV/atom) and low-energy (10 eV/atom) cluster ions. Using the spectral function of roughness, a highly efficient smoothing of the surface of nanostructured thin films of aluminum nitride was demonstrated in a wide range of spatial frequencies (ν = 0.02–128 μm-1) and at small etching depth (<100 nm).