Modern xerographic systems involve the integration of mechanical, electronic, software, and materials subsystems. Designing materials for this technology presents a number of challenges in which computational chemistry methods have played an increasingly important role in recent years. In this paper we will outline several examples where molecular level simulations have helped to develop fundamental insights into material structure/property relations and to establish design rules based on computable molecular properties and their relationship to appropriate end use requirements. The paper presents very brief highlights of our accomplishments in the areas of photogenerator pigments and polymers. In addition, it provides a brief commentary on how we approached the integration of simulation methodology into what has traditionally been an experimental environment.