Significant progress is being made in the photovoltaic energy conversion using organic semiconducting materials. One of the focuses of attention is the nanoscale morphology of the donor-acceptor mixture, to ensure efficient charge generation and loss-free charge transport at the same time. Using small molecule and polymer blend systems, recent efforts highlight the problems to ensure an optimized relationship between molecular structure, morphology and device properties. Here, we present two examples using a host/guest mixture approach for the controlled, sequential design of bilayer organic solar cell architectures that consist of a large interface area with connecting paths to the respective electrodes at the same time. In the first example, we employed polymer demixing during spin coating to produce a rough interface: surface directed spinodal decomposition leads to a 2-dimensional spinodal pattern with submicrometer features at the polymer-polymer interface. The second system consists of a solution of a blend of small molecules, where phase separation into a bilayer during spin coating is followed by dewetting. For both cases, the guest can be removed using a selective solvent after the phase separation process, and the rough host surface can be covered with a second active, semiconducting component. We explain the potential merits of the resulting interdigitated bilayer films, and explore to which extent polymer-polymer and surface interactions can be employed to create surface features in the nanometer range.