This work presents a systematic study of the effect of ZnSe nanocrystals (NCs) concentration on the optical and luminescent properties of poly N-vinylcarbazole (PVK) polymer nanocomposites. The ZnSe nanocrystals were synthesized by a simple co-precipitation chemical route, while PVK:ZnSe nanocomposite films were fabricated using the spin coating technique. The samples were characterized by XRD, TEM, SEM, UV-Vis and fluorescence techniques. The X-ray diffraction and TEM studies confirmed the particle size, microstructure and spherical shape of the synthesized nanocrystals. The ZnSe nanocrystals in PVK caused a decrease in optical gap with increasing concentration of nanocrystals. The emission spectra exhibited augmentation in intensity up to 70 wt.% of nanoparticles while further addition resulted in a decrease in luminescence. The structure-property relationships obtained for the present system are important for developing low cost illumination devices.