Sisal fibers were mercerized, under tension and no tension, to improve their tensile properties and interfacial adhesion with soy protein resin. Mercerization of fibers under tension is known to minimize fiber shrinkage and to lower the microfibrillar angle by aligning them along the fiber axis. Mercerization improved the fracture stress and Young’s modulus of the sisal fibers while their fracture strain and toughness decreased. Mercerized sisal fiber-reinforced composites with soy protein resin showed improvement in both fracture stress and stiffness by 12.2% and 36.2%, respectively, compared to the unmercerized fiber-reinforced composites. Scanning electron microscope (SEM) photomicrographs of the composite fracture surfaces showed shorter fibrils protruding in the mercerized fiber-reinforced composites resulting in better sisal fiber/soy adhesion. Changed fiber surface properties were also responsible for better adhesion.