The realization of semitransparent photovoltaics (ST-PVs) with optimal power conversion efficiency (PCE) and visible light transmittance (VLT) is an important step toward new applications such as power-generating windows for buildings and automobiles. A high-performing ST-PV should be wavelength selective, which best utilizes the ultraviolet (UV) and near-infrared (NIR) photons for photocurrent generation while balancing the absorption and transmission of visible photons. Semitransparent organic solar cells (STOSCs), coupled with wavelength-selective, one-dimensional photonic crystals (PCs), can meet such criteria, as organic semiconductors can achieve localized NIR absorption and PCs can further optimize device optical properties. Herein, by introducing a high-throughput optical model, we simulated over tens of millions of device configurations for PC-enhanced STOSCs to investigate their optical properties. Computationally guided fabrication of PC-enhanced PTB7-Th:IEICO-4F STOSC exhibited nearly 11% PCE and 30% VLT. The results exhibit the wide potential applications of high-throughput optical engineering, especially as related to designs including multi-objective and multi-layer thickness optimizations.