Shape memory composites (SMCs) combine mechanical performances of composite materials with functional behavior of shape memory polymers. They can be used to produce the external frame of self-deployable solar sails with very low weight in comparison with traditional composite booms. Furthermore, heat activation is necessary for deploying instead of complex mechanical devices. In this study, the mechanical behavior of a solar sail with SMC frame is simulated by means of finite element modeling. Design considerations are made on sail deployment configuration, size/weight ratio of solar sails, and SMC properties. An experimental activity has been also performed to provide suitable candidates for the composite laminates of the SMC structure. Mechanical and instrumented recovery tests have been carried out on 2-plies carbon-fiber laminates with a shape memory interlayer.