Recently, there has been an explosion of literature dedicated to organic electrodes for energy storage applications. While inorganic materials, especially oxides, have generally being explored for these applications, the guiding principles for successful electrical energy storage-maximizing capacity and energy density per unit mass and cost-have naturally led to the pursuit of organic materials. However, there has only been a modest focus on methods for systematic exploration, which could help establish rational design principles for their enhanced properties and performance. We will present computational and electrochemical studies for both pseudocapacitive cathodes based on conducting polymers with pendant redox sites, as well as Li-carboxylate materials for application as Li-ion anodes. We have previously demonstrated that the addition of a pendant charge storage component to conventional conducting polymer cathodes provides a significant increase in the capacity, in addition to well-defined voltage plateaus, all the while maintaining the superior rate capability of these materials. Explorations related to structure-property relationships in the conducting polymer backbone and redox pendant, and chemical stability of the pendant, indicate that these components are independently addressable, tunable through structural modifications, and that "ideal" high energy, highrate and high-cyclability organic materials can be realized. Further studies on Li-carboxylate anodes begin to elucidate the major structural features that dictate the redox, solubility and chemical reactivity properties of this promising class of organic electrode materials.