The application of chlorosomes, supramolecular antennae found in green photosynthetic bacteria, to the fabrication of hybrid nano-bio devices for solar energy applications has gained attention because of the potential of chlorosomes to harvest light even in low-light conditions and their resistance to harsh environments. The size of chlorosomes affects the exciton diffusion length in the antenna. In addition, combination of chlorosomes with nanostructured oxide films requires the assembly of chlorosomes in a specific orientation in order to successfully transfer the harvested energy into the oxide material. To do this effectively, it is essential to characterize the chlorosomes with respect to their size and charge distributions. In this work, chlorosomes from the green bacteria Chloroflexus aurantiacus were electrosprayed and their size was measured online in real-time using a rapid and precise mobility-based technique. Further, chlorosomes were electrospray-deposited onto TiO2 nanostructured films to explore the fabrication of low-cost efficient nano-bio devices.