Thin polymer films find diverse applications, from functional coatings like superhydrophobic surfaces to electrochemical technologies such as photovoltaics. With more applications and an increase in demand for said applications, there is a need to develop a cost-effective, high-precision, and high-throughput manufacturing process to produce thin polymer films and coatings with desired properties (e.g., morphology, composition). In our previous work, we introduced a simple and cost-effective approach, the air-assisted electrospray method, for surface coatings. Here, we expand on that foundation by exploring its capabilities for producing coatings with a wider range of surface morphologies and the fundamental understanding of the process. Through systematic control of concentration, needle configuration, and polymer selection, we achieve controlled coating morphologies from films to hybrid structures. Notably, the introduction of air assistance through a coaxial needle enhances the range of achievable morphologies, particularly at lower concentrations, and partially disrupts traditional electrospinning, showing results of simultaneous instances of electrospinning and electrospray. Furthermore, we demonstrate its broad application potential in the fabrication of binderless electrodes for battery applications.
