Monolayer and multilayer films were formed by electrostatic self- assembly of poly (allyl amine) hydrochloride (PAH) and a strong fluorescent dye eosin Y (EY). In agreementwith other published results, these compounds were found to form high-quality, closely packed monolayer and multilayer onto quartz substrate. The films formed on quartz substrate were then characterized in light of UV-Visible (UV-Vis) absorption spectroscopy and scanning electron microscopic (SEM) methods. Molecular movements were found to persist in the recently lifted layer-by-layer (LBL) films and about 72 h were required to get the film in stable condition. The photophysical characteristics of LBL films were found to vary with various parameters, such as number of deposited layers, dipping time in dye solution, pH of the PAH solution, and concentration of the dye. Both UV-Vis absorption spectroscopy and SEM studies also revealed the formation of molecular aggregates in the films.