underway to construct hydrogel materials into different shapes such as 3D, [5] 2D, [6] or fiber-like configurations, [7] wherein hydrogel fibers as a novel type of materials cast great impact on our daily life, ranging from smart textile, [8] conductor to functional reinforcements. [9] Compared with 3D and 2D hydrogels, fiber-like hydrogel, also known as 1D hydrogel fiber, always possess smaller cross-sectional areas, [10] which means such thin hydrogel fibers would bear more significant tensile force under the same load, leading to a higher standard on the mechanical properties for engineering 1D hydrogel fibers.With the synergistic effect of covalent and reversible bonds including hydrogen bonds, [11] hydrophobic interactions, [12] ionic bonds, and host-guest interactions, [13] a variety of hydrogel fibers with great mechanical properties have been developed, such as artificial spider silk with twisted core-sheath hydrogel fibers (tensile strength of 895 MPa and strain of 44.3%), [14] ultrastretchable fibers (tensile strength of 5.6 MPa and strain of 1180%), [9] and supramolecular fibers (tensile strength of 193 MPa and strain of 36%). [15] Despite their excellent mechanical properties, those hydrogel fibers are fabricated by manual drawing from the hydrogel, limiting their practical applications where scaled-up manufacture of fibers is required.To satisfy the demand of scaled-up production, the eligible hydrogel fibers are anticipated to be manufactured on a large scale via spinning process, including electrospinning, [16] extrusion spinning, [17] microfluidic or draw-spinning process. [18] For example, Ju et al. developed a hydrogel microfiber based on a continuous draw-spinning process, and the resulting fibers exhibited tensile stress of 1.4 MPa. [19] Song et al. spun a transparent hydrogel fiber possessing tensile stress of 200 kPa. [20] It should be noted that, as for spinning those hydrogel fibers, relatively low crosslinking density is often essential to a spinning solution due to the large deformation required during the spinning process and the requirements for spinning long and uniform hydrogel fibers, [19] which, in turn, leads to unsatisfied mechanical properties of the final spun hydrogel fibers.