The growth of nanocrystalline PbS films by chemical bath deposition (CBD) onto glass at temperature is presented in this research. We report on the modification of structural, optical, and electrical nanostructures due to in situ Ni-doping. The morphological changes of the layers were analyzed using SEM, AFM, and TEM. XRD spectra displayed peaks at 2θ = [26.00, 30.07, 43.10, 51.00, 53.48], indicating growth on the zinc blende face. The grain size determined by X-rays diffraction of the undoped samples was 36 nm, whereas with the doped sample was 3.2–5 nm. By TEM, the doped PbS was found crystalline films in the range 3.5–5 nm. Optical absorption (OA), and forbidden bandgap energy shift disclose a shift in the range 2.1–3.8 eV. Likewise, the dependence of with the radius size and interplanar distance of the lattice is discussed. Raman spectroscopy (RS) exhibited an absorption band 135 cm−1 displaying only a PbS ZB structure. The thermal energy for the films was determined from the slope of dark conductivity (DC) and the energy was estimated to be 0.15 to 0.5 eV.