Chitin, a high molecular weight (MW) linear polymer composed of N-acetyl-D-glucosamine (N-acetyl-2-amino-2-deoxy-D-glucopryanose) units linked by β-D (1→4) bonds is the second most abundant organic material after cellulose. Chitosan is the N-deacetylated derivative of chitin. Both of these biopolymers are intrinsically biocompatible and biodegradable, have aqueous adsorption capabilities, and chelate metals. Depending on the source of extraction, chitin exists in two crystalline polymorphic forms. Crustacean shells and butterflies contain α-chitin, whereas the polymorph β-chitin is more rare and found in squid pens. Electrospinning these biopolymers or biopolymer-composite mats could create flexible, affordable filtration membranes sensitive to metal ions or gas permeation. We have electrospun practical grade α-chitin as well as practical grade, low MW, medium MW, and high MW α-chitosan into non-woven mats. Two methods of cross-linking through the amine groups of chitosan were also employed to obtain an improved chemical stability. Chemical, morphological, and crystallinity analyses have been conducted utilizing FTIR, SEM, and XRD. To determine the metal absorption and mechanical properties of the mats, EDS and Kawabata microtensile testing were utilized, respectively. Despite the initial success with α-chitin, β-chitin has yet to be electrospun. Conductivity and rheology analysis, as well as the previously mentioned techniques are utilized to investigate and understand the differences between the polymorphic forms.