In this research, physical properties of nickel oxide nano-structured layers doped with various amount of Cu atoms (20–60 at.%) is studied using spray pyrolysis method on the glass substrate. The FESEM images show formations of nanostructures of about 20–60 nm and the XRD patterns show layers have a polycrystalline cubic structure nature with (111) as the preferred direction that its intensity reduces as the doping density increases. Analyzing transmittance UV. Vis spectra shows the variations of optical band gap of the samples are due to occurrence of doping atoms and quantum confined effects. Optical permittivity of different doped films have been compared using new numerical method and show the prominent effect of doping percent to real and imaginary parts of electrical permittivity. Also Hall effect results shows that Cu atoms substituted by Ni atoms sites play as acceptor atoms in the crystalline lattice. Finally, thermo-optical properties of the films have been studied using Nd–YAG laser illumination.