In article number 2001993, Kosuke Okeyoshi, Tatsuo Kaneko, and co-workers report that a cyanobacterial polysaccharide, sacran, is capable of flexibly transforming from straight microfiber into two-dimensional snaking and three-dimensional twisted structures. Furthermore, a vapor-sensitive film with a millisecond-scale response is developed by using the spring-like behaviour of twisted fibers. Such a unique fiber will establish a novel approach to the design of environmentally adaptive materials for soft sensors and actuators.