In this paper, nanostructured Ni-ZnS nanocatalysts were synthesized through a facile microwave combustion route. Powder XRD, FT-IR, EDX and SAED patterns revealed the presence of material in well crystalline single phase with average crystallite size of about 15 nm and the material remained cubic over the whole Ni-ZnS. Formation of ultrafine, spherical and homogeneous dispersed NPs with size 20 nm was confirmed by SEM and TEM analysis. VSM results confirmed a weak superparamagnetic behavior of Ni-ZnS and the values of Ms gradually increased with increasing the concentration of Ni2+ cations. The room temperature PL spectra of Ni-ZnS NPs showed extra peaks in yellow–orange and red region in comparison of undoped ZnS NPs. PL spectra was suggested with the significant enhancement of the PL intensity in Ni-ZnS NPs, due to Ni2+ incorporation.