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Chitin is a natural polysaccharides having a unique molecular arrangement of 2-(acetylamino)-2-deoxy-d-glucose, it possesses multifunctional properties and is suitable for various applications mainly in pharmaceutical, biomedical food, textiles and packaging fields. Therefore, being considered as a superior material for a sustainable future of industrial development, chitin perfectly meets up the demands with diversified functionalities in applications, excellent biocompatibility and biodegradability. Non-toxicity to human and environment (air, water and soil) is a great opportunity for this revolutionary, innovative and sustainable material. Moreover, antibacterial potency and low immunogenicity of chitin have broadened the aspects of research and development on structure-function relationship toward biological tissues and activities. Despite abundance, low cost and availability, many experimental data from potential studies, reproducibility problems of chitin solubility measurement still limit the development of products and access to the market in large volume. Batch-to-batch variability, non-precise characterization and randomly distributed acetyl groups of chitin structure eventually results in a bad reproducibility of chitin solubility. Therefore, the chapter aims to organize the information of chitin structure at molecular level and correlate solubility with chitin structure. Moreover, the dissolution mechanism and solution behaviors in different solvents will be discussed in this chapter.