This work focuses on the thermomechanical characterization and constitutive model calibration of shape memory polymers (SMPs). These polymers have the ability to recover seemingly permanent large deformations under the appropriate thermomechanical load path. In this work, a contribution is made to both existing experimental and modeling efforts. First, an experimental investigation is conducted which subjects SMPs to a thermomechanical load path that includes varying the value of applied deformations and temperature rates. Specifically, SMPs are deformed to tensile extensions of 10% to 100% at temperature rates varying from 1 degree C /min to 5 degree C/min, and the complete shape recovery profile is captured. The results from this experimental investigation show that the SMP in question can recover approximately 95% of the value of the applied deformation, independent of the temperature rate during the test. The data obtained in the experimental investigation are then used to calibrate, in one-dimension, two constitutive models which have been developed to describe and predict the material response of SMPs. The models include a model in terms of general deformation gradients, thus making it capable of handling large deformations. In addition, the data are used to calibrate a linearized version of the constitutive model for small deformations. The material properties required for calibrating the constitutive models are derived from portions of the experimental results, and the model is then used to predict the shape memory effect for an SMP undergoing various levels of deformation. The model predictions are shown to match well with the experimental data.