Composites were made from polyethylene and an organic fiber (pecan shell and peanut hull flour) using a compression-molding technique. Studies of variations in molding temperature (145–180°C), fiber concentration (0–40% by weight), and fiber mesh size (100, 200, and 325) were correlated to the mechanical properties of the composites (tensile strength, elongation, fracture energy, modulus, and impact strength). In untreated nut shell composites, tensile strength decreased steadily as the fiber concentration increased. This was due to poor bonding between the untreated fiber and polymer. Polyisocyanate was used as a coupling agent and its effect on mechanical properties of the composites was studied. Significant improvement in tensile strength was achieved with an isocyanate coupling agent, but it had no effect on modulus of the composites. Both untreated and isocyanate-treated composites had lower impact strength values; further composite matrix modifications would be necessary to maintain or improve impact strength.