We have found a correlation between ZnS nanocomposite nonlinear optical features and technological processing using electrolytic method. In the earlier researches this factor was neglected. However, it may open a new stage for operation by photovoltaic features of the well known semiconductors within a wide range of magnitudes. The titled nanostructured zinc sulfide (ZnS) was synthesized by electrolytic method. The obtained ZnS nano-crystallites possessed nano-particles sizes varying within 1.6nm…1.8nm. The titled samples were analyzed by XRD, HR-TEM, STEM, and nonlinear optical methods such as photo-induced two-photon absorption (TPA) and second harmonic generation (SHG). For this reason the nano-powders were embedded into the photopolymer poly(vinyl) alcohol (PVA) matrices. Role of aggregation in the mentioned properties is discussed. Possible origin of the such correlations are discussed.