Producing novel functional nanomaterials with high reproducibility is extremely desirable but very challenging. Further treatment by reliably combining or embedding nanoparticles (NPs) into a protecting medium could be a promising approach to retaining their properties and realizing practical applications. In this work, we report the preparation, characterization, and potential applications of flexible and selfstanding polymer nanocomposite films embedded with ZnO:Tb 3+ nanophosphors suitable for optical devices. The nanocomposite films were prepared from ZnO:Tb 3+ phosphor NPs synthesized by a solution combustion method and a solution of polystyrene (PS) in toluene. The structural, morphological, thermal, and optical properties of phosphor polymer nanocomposite (PS/ZnO:Tb 3+ ) films were studied. These studies showed that the ZnO:Tb 3+ phosphor NPs were uniformly distributed throughout the polymer films, providing higher stability to the thermal and photoluminescence (PL) properties of the films. The PL properties of the nanocomposite films increased with an increase in the nanophosphor concentration. The temperature-dependent PL properties of the PS/ ZnO:Tb 3+ films were also studied. This study reveals that the embedded nanophosphor NPs retain their unique luminescent properties without any significant spectral shift, indicating their potential applications in solid-state lighting.