Smart materials and structures have developed rapidly, especially their application in the aerospace field has been widely valued and recognized in recent years. Shape memory cyanate ester (SMCE) resin as a class of smart polymers has a broad application prospect in space deployable structure due to the high glass transition temperature (Tg) and excellent mechanical properties. In this work, the high storage modulus SMCE resins were prepared by regulating cyanate prepolymer with small molecules, showing high glass transition temperature (Tg > 218℃), high Young’s modulus (E’ > 3.15 GPa), and outstanding γ-ray radiation resistance. The SMCE resins maintained a high shape fixity rate (Rf > 95 %) at high operating temperatures (100 ℃ and 120 ℃) for 30 days, providing a great potential application for active deformation structures. Moreover, the synergy of carboxyl (-COOH) functionalized multi-walled carbon nanotubes (CNT) and short carbon fibers (CF) enhanced the thermodynamic properties and shape-changing function of the SMCE composites. The spring made by SMCE composite exhibits 360° freedom rotation, which can be used as smart structures in the aerospace field.