Sisal fiber was treated by admicellar polymerization with a poly(methyl methacrylate) film coating in order to enhance the interfacial adhesion of the fiber/polymer composite for mechanical property improvement. Properties of the admicellar-treated sisal fiber were investigated by measuring its moisture absorption and electrostatic charge. Thermal stability study by thermogravimetric analysis and film identification by FTIR was also carried out. The treatment was shown to improve the tensile and flexural properties, impact strength, and hardness of the composite. SEM micrographs of the tensile fracture surface of sisal/unsaturated polyester composites also show interfacial adhesion improvement of the composite prepared with admicellar-treated sisal.