Chitin and chitosan exhibit immense potential purposes as biomaterials, wearable versatile digital gadgets, power conversion and storage supplies, and meals packaging. Nonetheless, the event of a common inexperienced aqueous solvent for chitin and chitosan, and a complete understanding of their dissolution mechanism, requires additional investigation. Right here, the fast dissolution of chitin and chitosan with diploma of deacetylation lower than 80% within the common solvent KOH/urea aqueous answer has been analyzed. The hierarchical structural transitions and interactions of deacetylated α-chitin and chitosan within the KOH/urea aqueous answer have been investigated. Subsequently, a desolvation-intercalation dissolution mechanism was proposed. This research may information future analysis on chitin and chitosan on the molecular degree, facilitating the event of superior chitin- and chitosan-based supplies with purposes starting from bioelectronics to regenerative medication.