DIW 3D Printing Aligned Catkins to Access Significant Enhanced Responsive Ionogel

Although stimuli‐responsive gels have received significant attention due to their flexible structure and high tolerance to various stimuli, the high solvent content leads to relatively low mechanical properties and instability in performance due to water evaporation. This limits their application to some extent. Here, catkins enhanced ionogel is crafted that prevents solvent vaporization‐induced properties from abating yet remains humidity responsiveness. By using direct ink writing (DIW) 3D printing, the catkins can be aligned within the ionogel, resulting in a significant increase in ionic conductivity (0.17 S·cm−1) and mechanical properties (4.75 times). Moreover, the environment stability (−50–150 °C) and hygroscopicity of the ionic liquid (IL) allow the 3D‐printed composite to perform a controllable lubrication behavior in response to changes in humidity and temperature. This work demonstrates the significant enhancement of responsive ionogels through DIW 3D printing with aligned catkins and presents a new strategy for achieving the lubricating regulation. In this study, DIW 3D printing is used to align the catkins and create an anisotropic structure of the ionogel. The resulting anisotropic structure shows significant differences in mechanical properties and ionic conductivity.