Our modern lives and related environmental concerns dictate the growing demand for renewable and non-polluting energy sources, and therefore, considerable effort is being employed to harness natural resources, in particular sunlight, for energy production. Solar energy can be used directly as thermal energy or converted to electricity using photovoltaics materials. Thus, researchers are pursuing new materials that can provide current upon light illumination. Natural light-harvesting complexes, such as the photosystem (PS), drew some attention in this direction because of their natural function in producing energy upon light excitation. Previous studies revealed the possibility of generating photocurrents using the PS protein and of utilizing the protein in photovoltaic devices and solar cells. The use of the PS protein in such devices requires a deposition process of the PS, resulting in a monolayer or a multilayer film, and thus, it has to be formed on a surface, such as an electrode or gold nanoparticle. Furthermore, in most studies the photocurrent generation was achieved in an electrochemical setup, i.e., in an aqueous solution, which can be a limiting factor. In natural systems, the light energy is harvested by a myriad of chromophores situated within proteins, one of the most common ones of which is the chlorophyll (Chl) chromophore. Chl by itself was also tested for its ability to serve as a light-harvesting moiety, where a monolayer or multilayers of Chl were deposited on metal or semiconducting electrodes, resulting in photocurrent generation in a photoelectrochemical setup. Inspired by the natural role of the PS, we designed in this study a synthetic free-standing proteinbased polymeric platform that facilitates photocurrent production. The platform is based on electrospun bovine serum albumin (BSA) mats that were molecularly doped with Chl chromophores.