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Luminescent polymethylmethacrylate (PMMA) films were prepared by the solvent-casting technique from polymer solution doped with different concentrations of red perylene dyestuffs (KREMER 94720 and KREMER 94739). The effect of the dye concentration on the structure and spectroscopic properties was studied using X-ray diffraction (XRD), transmission electron microscope (TEM) optical absorption, and fluorescence spectroscopy. The optimum dye concentration of photoselective PMMA films was determined by the fluorescence spectroscopy measurements and showed the best emission properties for the doping concentration 10−3 wt % of the investigated dyes. The accelerated photostability tests showed promising stability of the prepared films towards terrestrial solar ultraviolet radiation (UVA). The results endorsed a promising application of the investigated films in photoselective greenhouse cladding applications as the optimized film fluoresces at the action spectra of special chlorophyll a.