Due to their potential for solar energy harvesting and storage, molecular solar thermal energy storage (MOST) materials are receiving wide attention from both the research community and the public. MOST materials absorb photons and convert their energy to chemical energy, which is contained within the bonds of the MOST molecules. Depending on the molecular structure, these materials can store up to 1 MJ/kg, at ambient temperature and with storage times ranging from minutes to several years. This work is the first to thoroughly investigate the potential of MOST materials for the development of energy saving windows. To this end, the MOST molecules are integrated into thin, optically transparent films, which store solar energy during the daytime and release heat at a later point in time. A combined experimental and modeling approach is used to verify the system's basic functionality and identify key parameters. Multi-physics modeling and simulation were conducted to evaluate the interaction of MOST films with light, both monochromatic and the entire solar spectrum, as well as the corresponding dynamic energy storage. The model was experimentally verified by studying the optical response of thin MOST films containing norbornadiene derivatives as a functional system. We found that the MOST films act as excellent UV shield and can store up to 0.37 kWh/m2 for optimized MOST molecules. Further, this model allowed us to screen various material parameters and develop guidelines on how to optimize the performance of MOST window films.