Neodymium-doped polyvinyl alcohol films were prepared and the optical properties of the films were investigated. By applying Judd-Ofelt theory, the X parameters were obtained from the absorption spectrum. Various radiative parameters like transition probability for each level (A J ), total transition probability (A T ), branching ratio (b R ), radiative lifetime (s rad ), and absorption cross-section (r A ) were calculated. The theoretically obtained branching ratio and integrated absorption cross-section are found to be greater for the transition 4 F 3/2 ! 4 I 11/2 . From the emission spectrum peaked at 1064-nm stimulated emission cross-section (r E ), the line width (Dk eff ) is calculated to be 6.21 Â 10 À21 cm 2 and 41 nm, respectively. Further the variation of the optical gain with the length of the film was studied and the slope efficiency (g ¼ 8.5%) was determined from laser measurements. These results clearly support the potentiality of the Nd 3þ : polyvinyl alcohol films in realizing optical amplification and stimulated emission.