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The power conversion efficiency of polymer solar cells today has passed 10%, the commonly acceptable value for commercial usage. However, in general labs, the power conversion efficiency routinely achievable is only at 3–5% because of the lack of effective tools to optimize the device design and the fabrication process. Instead of using trial-and-error experiments to improve the power efficiency, modeling and simulation provides an alternative, effective, and economical way to optimize the design of polymer solar cells for best device performance. This review gives a literature survey, including some of our own studies, on modeling and simulation of polymer solar cells. First, the fundamentals of polymer solar cells are briefly explained. Then, the optical and electrical modeling and simulation are discussed in detail, followed by a discussion on optimization of polymer solar cells via modeling and simulation. This review ends with an outlook for the future study on modeling, simulation, and optimization of polymer solar cells.