Shape‐memory polymers (SMPs) are smart, responsive materials with numerous potential applications. Based on previously introduced shape‐memory natural rubber (SMNR), which shows exceptional properties such as strain storage of 1000%, cold storage, cold programmability, and mechanical and thermal triggers tunable both during and after programming, different SMNRs regarding their shape‐memory parameters are investigated. Furthermore, their energy‐storage capability and their mechanical properties are explored. SMNRs show fixity ratios of up to 94% and excellent recovery ratios of up to 100% whereas strains even above 1000% can be stored. Energies of up to 4.88 J g−1 can be stored with efficiencies of up to 53.30%. Further, the Young's modulus of SMNR can be switched by two orders of magnitude upon triggering or programming.
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