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Atmospheric water vapor is an abundant and renewable resource that can alleviate growing water scarcity. Hybrid hydrogel desiccants composed of hygroscopic salts hold significant promise for atmospheric water harvesting (AWH) due to their increased capacity for water uptake. Thus far, many efforts in fabricating these desiccants require multistep processes, where the salt impregnation is achieved post-hydrogel fabrication. Here, we develop a scalable wet spinning methodology using aramid nanofibers (ANFs) to template and coagulate hydroxypropyl cellulose (HPC) into filaments in a coagulation bath consisting of water and lithium chloride (LiCl). HPC serves as the matrix to retain the captured water vapor, and later releases it upon heating. ANFs serve as the physical cross-linker between HPC, allowing for wet spinning at a speed up to 61 m h–1. The composite filaments achieve up to 0.55 g g–1 water uptake at 30% relative humidity (RH) and 21 °C, reaching 80% saturation in 40 min. With a lower critical solution temperature of 39 °C, the desiccant filaments can release up to 72% of the captured water at 60 °C after 30 min. In an AWH chamber, the filaments can achieve daily water production of 5.21 L kg–1 day–1 at 30% RH and 21 °C. 

Abstract Cholesteric liquid crystal elastomers (CLCEs) hold great promise for mechanochromic applications in anti‐counterfeiting, smart textiles, and soft robotics, thanks to the structural color and elasticity. While CLCEs are printed via direct ink writing (DIW) to fabricate free‐standing films, complex 3D structures are not fabricated due to the opposing rheological properties necessary for cholesteric alignment and multilayer stacking. Here, 3D CLCE structures are realized by utilizing coaxial DIW to print a CLC ink within a silicone ink. By tailoring the ink compositions, and thus, the rheological properties, the cholesteric phase rapidly forms without an annealing step, while the silicone shell provides encapsulation and support to the CLCE core, allowing for layer‐by‐layer printing of self‐supported 3D structures. As a demonstration, free‐standing bistable thin‐shell domes are printed. Color changes due to compressive and tensile stresses can be witnessed from the top and bottom of the inverted domes, respectively. When the domes are arranged in an array and inverted, they can snap back to their base state by uniaxial stretching, thereby functioning as mechanical sensors with memory. The additive manufacturing platform enables the rapid fabrication of 3D mechanochromic sensors thereby expanding the realm of potential applications for CLCEs.