In the present investigation, at first, the surface of zinc oxide (ZnO) nanoparticles was treated with a silane coupling agent of gamma-methacryloxypropyltrimethoxy silane (KH570), which introduces organic functional groups on the surface of ZnO nanoparticles. Secondly, optically active poly(amide-imide) (PAI) was synthesized via solution polycondensation of N,N'-(pyromellitoyl)-bis-phenylalanine diacid chloride 1 (M-1) with 4,4'-diaminodiphenylsulfone 2 (M-2). The polycondensation of diacid chloride with aromatic diamine was carried out with N,N-dimethylacetamide/triethylamine systems. Finally PAI/ZnO nanocomposites (NCs) containing 4, 8, and 12% of nanoparticles were successfully fabricated through ultrasonic irradiation technique. The obtained NCs were characterized by Fourier transform-infrared (FT-IR) spectroscopy, thermogravimetry analysis, X-ray powder diffraction, UV-Vis spectroscopy, scanning electron microscopy (SEM), field emission-scanning electron microscopy (FE-SEM), and transmission electron microscopy (TEM). The FT-IR spectroscopy indicated that the silane coupling agent was anchored on the surface of ZnO nanoparticles. SEM, FE-SEM, and TEM images were showed ZnO nanoparticles were dispersed homogeneously in PAI matrix.