Electrospinning is a complex process that requires numerous interacting physical instabilities. Assuming that a chosen polymer and solvent system can be spun, the chosen polymer exists in various states, which have variable crystallinities starting with the highest degree of crystallinity (when in bulk form) and ultimately being transformed into a non-woven mat. In an effort to better understand the effects that the electrospinning process has on the biopolymers chitin [practical grade (PG)] and chitosan [PG and medium molecular weight (MMW)], including post-production neutralization and cross-linking steps, field emission scanning electron microscopy (FESEM) and solubility studies were performed. An evaluation of diffraction peaks of the bulk, solution, and fibrous forms of chitin and chitosan were evaluated by X-ray diffraction (XRD) and determined that the formation of chitosan chains is influenced by the addition of solvent and cross-linking agent. This study is of importance since the crystallinity of chitin and chitosan directly relate to the ability of the biopolymers to chelate metals, and the chemical stability of non-woven mats aid in the creation of functional filtration membranes.