This paper considers the design of spatially varying porosity profiles in next-generation electrodes based on simultaneous optimization of a porous-electrode model. Model-based optimal design (not including the solid-phase intercalation mechanism) is applied to a porous positive electrode made of lithium cobalt oxide, which is commonly used in lithium-ion batteries for various applications. For a fixed amount of active material, optimal grading of the porosity across the electrode was found to decrease the ohmic resistance by 15%-33%, which in turn increases the electrode capacity to hold and deliver energy. The optimal porosity grading was predicted to have 40% lower variation in the ohmic resistance to variations in model parameters due to manufacturing imprecision or capacity fade. The results suggest that the potential for the simultaneous model-based design of electrode material properties that employ more detailed physics-based first-principles electrochemical engineering models to determine optimal design values for manufacture and experimental evaluation. (C) 2010 The Electrochemical Society. [DOI: 10.1149/1.3495992] All rights reserved.