As a green bioresource, cellulose nanocrystal (CNC) offers enormous chemical, material, and food industry opportunities. By manipulating the interactions in CNC-based suspensions, we developed hydrogels with appropriate rheological properties required for 3D extrusion printing. To achieve this, we utilized a wide range of salts (NaCl, KCl, CaCl2, AlCl3, NH4Cl, CaSO4) featuring different sizes and ion strengths. Rheological properties showed that the hydrogel's dynamic shear moduli enhanced with increasing charge and size of the cation at any given CNC concentration. In addition, the results showed that, regardless of salt type, hydrogels containing 5wt.% CNC and 200mM salts exhibited optimal printing quality, featuring a high aspect ratio (i.e., more than 20 3D printing layers). Generally, the existence of a salt with a higher charge number (AlCl3) and larger ionic radius (CaCl2) enhances the cross-linking of the hydroxyl groups, resulting in higher printing resolution. These high-quality 3D printed samples can be used in complex biomedical scaffolds.