Luminescent solar concentrators (LSCs) provide a simple and cost‐effective strategy for harvesting sunlight. However, few existing LSC–solar cell systems possess power conversion efficiency (PCE) and remarkable color rendering capability simultaneously, which limits their application in building‐integrated photovoltaics (BIPV). Herein, for the first time, novel LSC–solar cell systems fabricated by integrating LSCs with organic solar cells (OSCs), accompanied with efficient solar energy harvest and excellent color rendering, are reported. Three conjugated copolymers, PPF‐IF, PPF‐NIF, and PPF‐F are utilized as the luminophores to construct LSCs with ultrahigh color rendering indices (95.74), and the OSCs based on these systems present high PCEs (4.92%) under 1 sun conditions. With the decrease of the light intensity, the PCEs of the OSCs keep rising and reach a high value of 14.91% (11 mW cm−2). In contrast, the crystalline silicon (C–Si) cell‐based systems show low PCE values ranging from 1.90% to 2.47%, and especially, the PCEs are not highly correlated with the illumination intensity. These results indicate that the utilization of conjugated copolymers as luminophores can enable LSC to possess high efficiency and excellent color rendering ability, and the integration of OSCs with LSC is a very promising strategy for future practical applications in BIPV, etc.