Engineering the rheological properties of colloidal inks is one of the main challenges in achieving high-fidelity 3D printing. Herein, we provide a comprehensive study on the rheological behavior of inks based on cellulose nanocrystals (CNCs) in the presence of given salts to enable high-quality 3D printing. The rheological properties of the CNC suspensions are tailored by considering the nature of the electrolyte (i.e., 10 types of salts featuring different ion sizes, charge numbers, and inter- and intra-molecular interactions) at various concentrations (25-100 mM). A high printing fidelity is achieved in a narrow CNC and salt concentration range, significantly depending on the salt type. The structure-property relationship is explored in a "3D-printing" space (2D map), introducing a guideline for researchers active in this field. To further unravel the effect of salt type on morphological properties, CNC aerogels are developed by freeze-drying the printed structures. The results illustrate that enhancing viscoelastic properties render a denser structure featuring smaller pores.