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To unlock nature's potential for functional biomaterials, many efforts have been devoted to isolating the nanocrystalline domains within the supramolecular structure of polysaccharides. Yet, low reactivity and yield in aqueous systems along with excessive solvent usage hinders its development. In this report, the first solvent‐free pathway to access carboxylated chitin and cellulose nanocrystals with excellent mass balance is described, relying on a new method coined high‐humidity shaker aging (HHSA). The method involves a mild grinding of the polysaccharide with ammonium persulfate followed by an aging phase under high‐humidity and on a shaker plate. Insights into the mechanism were uncovered, which highlighted the unique role of high humidity to afford a gradual uptake of water by the material up to deliquescence when the reaction is complete. This process was then validated for direct synthesis of nanocrystals from biomass sources including crab and soft wood pulp. [ABSTRACT FROM AUTHOR]