The use of polymers in the fabrication of bilayers for stimuli-responsive systems is well-known, yet viscoelasticity and viscoelastic models representing bilayer behavior have received surprisingly little attention. Of particular recent interest to us are simple polymeric bilayers in which one material, such as styrene-ethylene-propylene-styrene (SEPS) or styrene-isobutylene-styrene (SIBS), shows typical rubbery elastic response upon extension and retraction, and the other, an unvulcanized, low-Tg polymer such as butyl rubber (butyl), exhibits a viscoelastic response. When such a bilayer strip is extended to a fixed strain and held for several seconds followed by sudden release of this strain, rapid curling is observed, achieving a maximum curvature within 1 second, with a gradual uncurling, typically taking 300-600 seconds to eventually return to a flat strip. Attention has been directed to modeling the observed bilayer behavior. We compare predicted curvature and relaxation time constants from finite element analysis (FEA) simulations using Maxwell, Zener, Generalized Maxwell, and Parallel Rheological Framework (PRF) viscoelastic models to the experimentally measured values. We find that the Generalized Maxwell model predicts curvature over time with the lowest overall mean absolute scaled error (MASE) of 0.519, corresponding to a 4.9% difference from the second lowest error model and a 76.8% difference from the highest error model. Building upon an understanding of the material mechanics in simple bilayer strips, more complex bilayer systems can be designed. Samples of cross and weave geometries were fabricated from bilayer films and initial testing demonstrates how these materials can be used in potential applications.