AbstractMotile organs have evolved in climbing plants enabling them to find a support and, after secure attachment, to reach for sunlight without investing in a self-supporting stem. Searching movements, the twining of stems, and the coiling of tendrils are involved in successful plant attachment. Such coiling movements have great potential in robotic applications, especially if they are reversible. Here, the underlying mechanism of tendril movement based on contractile fibers is reported, as illustrated by a function–morphological analysis of tendrils in several liana species and the encoding of such a principle in a core–shell multimaterial fiber (MMF) system. MMFs are composed of a shape-memory core fiber (SMCF) and an elastic shell. The shape-memory effect of the core fibers enables the implementation of strain mismatch in the MMF by physical means and provides thermally controlled reversible motion. The produced MMFs show coiling and/or uncoiling behavior, with a high reversible actuation magnitude of ≈400%, which is almost 20 times higher compared with similar stimuli for sensitive soft actuators. The movements in these MMFs rely on the crystallization/melting behavior of oriented macromolecules of SMCF.