LAUSR

Nanocellulose has become an important renewable component for composite inks, owing to its desirable physical properties, reinforcing capabilities, and tunable self‐assembly behavior. However, it is difficult to improve the rheological performance of the nanocellulose‐based composite to meet the requirement for 3D printing high resolution microarchitectures. Herein, a strategy is proposed that incorporation of amphiphilic molecular surfactant into nanocellulose gel can increase the molecular interaction via hydrophobic bonds and enhance the ink viscoelasticity. Following the design, a composite ink is formulated by adding xylan and Nonaethylene glycol monododecyl ether (C12E9) within nanocellulose gel. A new printing program is designed to achieve vertical writing of the composite ink and obtain free‐standing micropillars and microhemispheres with high resolution in dozens of micrometers. The microhemisphere on an atomic force microscope (AFM) cantilever can be used as colloidal probe. This work proves that nanocellulose composite ink is a candidate for 3D printing functional devices with special microstructures.