We study large deformations of hyperelastic membranes using a purely two-dimensional formulation derived from basic balance principles within a modern geometric setting, ensuring a framework that is independent of an underlying three-dimensional formulation. To assess the predictive capabilities of membrane theory, we compare numerical solutions to experimental data from axisymmetric deformations of a silicone rubber film. Five hyperelastic models—Neo-Hookean, Mooney-Rivlin, Gent, Yeoh, and Ogden—are evaluated by fitting their material parameters to our experimental data using TensorFlow. Our results provide a systematic comparison of these models based on their accuracy in capturing observed deformations, establishing a framework for integrating theory, experiment, and data-based parameter identification.