Bioinks from All‐Natural Pickering Emulgels Co‐Stabilized by Cationic CNC and Inclusion Complexes Formed by α‐Cyclodextrin

Abstract Direct ink writing is especially relevant to the biomedical field due to the customizable extrusion and the possibility of creating pre‐designed architectures. Abundant natural polymers are sustainable and biocompatible alternatives to synthetic and persistent polymers. The printing of pure nanocellulose suspensions proves difficult due to low solid loadings, high shrinkage, as well as non‐fitting rheology. Emulsion gels (emulgel) alternatives gain attention in the field owing to their favorable viscoelastic properties and the possibility of creating multiphase systems. The authors’ sulfur‐free cationic cellulose nanocrystals (CNC) of low degree of substitution enable straightforward deployment in Pickering emulsions. An emulgel ink co‐stabilized by cationic CNC and α‐cyclodextrin is introduced as an interfacial inclusion complex. All ink components are natural and biodegradable compounds. The produced emulgel inks allow for high fidelity printing and minimum shrinkage upon drying that relaxes the need for supports, even in complex overhanging structures. A low yield stress (230–270 Pa) facilitates the inclusion of cells for biomedical applications into the formulation. The emulgel can be tuned to the desired rheological properties and be equipped with both polar and apolar compounds due to the biphasic system, making it a promising platform for biocompatible additive manufacturing.