The last few decades have witnessed a remarkable and positive contribution of biogenically synthesized biomaterials to modern medicine, most especially in the areas of regenerative medicine and drug delivery. By virtue of this development, notable successful applications of biogenic sutures and scaffolds for accelerated wound healing; novel drug delivery system for cancer immunotherapy and vaccines; and biomaterials for skin and bone replacement/repair in plastic/cosmetic surgery are now available in open literature for reference. Nonetheless, the list of these emergent materials is not yet exhaustive which translates to room for the development of more similar materials with improved properties. In light of this, the present study investigated the suitability and efficiency of enhancing the economic viability, structural integrity, hydrophilicity, abrasive wear behaviour, kinetics of moisture diffusion (in simulated body fluid) of polylactide with deacetylated chitosan extracted from crab’s exoskeleton. Prior to physical experimentation, numerical prediction of the miscibility of the two polymers under investigation was carried out to preview the feasibility of the research. Both molecular dynamics simulation and desired experimental techniques were used to develop and characterize the polylactide/chitosan composite materials.