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In this paper, we report an approach to polymerization of a nanocomposite containing UV-polymerizable organic material and inorganic, NaYbF₄:Tm³⁺ core-based nanoparticles (NPs), which are optimized for upconversion of near infrared (NIR) to ultraviolet (UV) and blue light. Our approach is compatible with numerous existing UV-polymerizable compositions and the NaYF₄: Yb, Tm³⁺ core-based NPs are much more stable against harsh conditions than NIR organic photo-initiators proposed earlier. The use of a core-shell design for the NPs can provide a suitable method for binding with organic constituents of the nanocomposite, while maintaining efficient NIR-to-UV/blue conversion in the NaYbF₄ core. The prepared photopolymerized transparent polymer nanocomposites display upconversion photoluminescence in UV, visible and NIR ranges. We also demonstrate a successful fabrication of polymerized nanocomposite structure with millimeter/submillimeter size uniformly patterned by 980 nm irradiation of inexpensive laser diode through a photomask.