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Energy harvesting devices based on a piezoelectric material attached to asymmetric bistable laminate plates have been shown to exhibit high levels of power extraction over a wide range of frequencies. This paper optimizes for the design of bistable composites combined with piezoelectrics for energy harvesting applications. The electrical energy generated during state-change, or “snap-through,” is maximized through variation in ply thicknesses and rectangular laminate edge lengths. The design is constrained by a bistability constraint and limits on both the magnitude of deflection and the force required for the reversible actuation. Optimum solutions are obtained for differing numbers of plies and the numerical investigation results are discussed.