The thin films of Nickel Phthalocyanine (NiPc) on glass substrates were prepared by vacuum evaporation at different substrates temperatures (300, 325, 350, 400, 450) K. The structure and surface morphology of NiPc in powder and thin film forms (265 nm) were studied using X-ray diffraction and atomic force microscope (AFM), and showed that there was a change and enhance in the crystallinity and surface morphology due to change in the substrates temperatures. Analysis of X-rays diffraction patterns of NiPc in powder form showed that it had an α-polycrystalline phase with monoclinic system with lattice constants a = 1.513 nm, b = 0.462 nm, c = 2.03 nm and β = 123.46°. Thermal evaporation of NiPc at different substrates temperatures led to β-crystalline films oriented preferentially to the (100) plane with different substrate temperatures. The mean crystallite size increased with substrates temperatures from 300 K to 450 K. This result was supported by AFM measurements, which exhibited a relatively larger grain size.