GeSe is a promising absorber material for photovoltaic applications due to its attractive material, optical, and electrical properties as well as its low toxicity and earth abundance. The first GeSe‐based solar cell with 1.48% efficiency has been recently reported through self‐regulated rapid thermal sublimation. However, most of the fundamental physical and electronic properties of GeSe such as refractive index, dielectric constant, carrier mobility, lifetime, and diffusion length remain unclear, despite the necessity of this for the design of high‐performance GeSe solar cells. In this work, the above basic properties of GeSe are systematically studied by using spectroscopic ellipsometry, space charge limited current measurements, and transient absorption spectroscopy. These comprehensive results provide a solid foundation for the further development of GeSe solar cells.