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Cellulose fibers are widely used as reinforcing fillers in composite materials. Many studies have been performed on biodegradable composites of poly(lactic acid) incorporating cellulose whiskers with the goal of improving physical properties. However, it is not easy to disperse the generally hydrophilic cellulose fibers uniformly in the hydrophobic polymer matrix. In this study, we proposed a novel way to incorporate cellulose fibers into poly(lactic acid) by functionalizing them with whole milk casein protein. Surface plasmon resonance studies showed strong interaction between whole milk casein and poly(lactic acid). Adsorption coefficient for the binding of poly(lactic acid) to casein surfaces was around 4104 M-1. The potential of using casein as an intermediate to increase the affinity of cellulose fibers to poly(lactic acid) is discussed.