To fabricate G/PVP/PANI nanocomposites on the paper-based biosensor, electrospraying is selected because a 3D droplet-like nanostructure can be created on the modified electrode surface. Compared to thin-film modified electrodes, G/PVP/PANI-nanodroplet-modified electrodes offer a higher specific surface area, which leads to an enhanced electrochemical sensitivity of the biosensors. Increasing the electrode surface area through this method might be very useful for further biofunctionalization, such as enzyme loading.