microfibrils are embedded. [10] These structures, which resemble artificial fiber-reinforced composites, deform largely along the alignment of the microfibrils, and deformation perpendicular to this reinforcement occurs less strongly. [11] This differential deformation is then transferred to macroscopic shape-shifting mechanisms such as self-winding. Self-winding is a competition between bending and twisting, which often stems from a need to release potential energy present in surface stresses, misfit strains, residual strains, thermal stresses, differential growth, shrinkage, or swelling. [12] Understanding these mechanisms is of fundamental importance to gaining insights into the design and application of helical shapes. Various works have been inspired by biological principles to generate self-winding as a response to external stimuli; however, most of them focus on the design of bilayers with mismatching properties. [11,13-15] Usually, the precursor is a flat ribbon or a straight rod formed by two layers with differential responses to stimuli. [3,16] However, simple formulation and production methods that mimic the spontaneous nature of self-coiling are still lacking. Here, we present a new fabrication approach that originates spontaneously self-winding wires upon their differential swelling in water. We apply biomimetic concepts to designing gelatin wires that are reinforced by amyloid fibrils (AFs) following principles similar to fiber-reinforced composites. Our fabrication dry-spins a single phase, thus bypassing the need for precise bilayer design and offering an easy, scalable, and sustainable alternative to more complex material designs. We employ β-lactoglobulin (BLG) to form AFs because of its rich and chiral structure. Although amyloid fibrils have promising properties, they alone cannot be processed as biopolymers because of their high rigidity and low plasticity. Therefore, we combine the plasticity of gelatin with the rigidity and versatile functionalization of AFs to produce wires that spontaneously self-wind in water. We investigate the origins of self-winding mechanisms by modeling the relative contributions of twisting and winding to the free energy. Finally, we explore the potential applications of such self-wound wires in sensors and actuators and complement our experimental results with theoretical interpretations. The wires disclosed here are, to the best of our knowledge, the first example of a system that is capable of performing as both actuator and sensor, produced entirely