We developed a 100 % bio-based pressure sensitive adhesive (PSA) possessing strong adhesion, as well as reusability, recyclability, and on-demand removability. The adhesive formulation is based on a colloidal mixture of starch (specifically amylopectin) nanoparticles and cellulose nanofibrils, combined with an aqueous solution of sorbitol and glycerol. Optimization of water supply and substitution of water with hygroscopic glycerol were implemented to address the challenges caused by the use of high water contents in hydrogels. By leveraging physical crosslinking through hydrogen bonding, we achieved high adhesion strength, reversibility, and reusability with 100% bio-based materials. The optimal formulation demonstrates excellent rheological and adhesion properties, which are comparable to petrochemical-based adhesives in terms of tack, peel strength, and shear strength. While there are areas for further optimization, this work provides a foundational step towards a more sustainable adhesive industry.