Neodymium-doped polyvinyl alcohol films were prepared and the optical properties of the films were investigated. By applying Judd-Ofelt theory, the Q parameters were obtained from the absorption spectrum. Various radiative parameters like transition probability for each level (A(l)), total transition probability (A(T)), branching ratio (beta(R)), radiative lifetime (tau(rad)), and absorption cross-section (sigma(A)) were calculated. The theoretically obtained branching ratio and integrated absorption cross-section are found to be greater for the transition F-4(3/2) -> I-4(11/2). From the eniission spectrum peaked at 1064-nm stimulated emission cross-section (sigma E), the line width (Delta lambda(eff)) is calculated to be 6.21 x 10(-21) 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 (eta = 85%) was determined from laser measurements. These results clearly support the potentiality of the Nd3+: Polyvinyl alcohol films in realizing optical amplification and stimulated emission. (C) 2009 Wiley Periodicals, Inc. J Appl Polym Sci 113: 887-895, 2009