DescriptionElectrospray deposition (ESD) is a spray coating process that utilizes a high voltage to atomize a flowing solution into charged microdroplets. These self-repulsive droplets evaporate as they travel to a target substrate, depositing the solution solids. Past ESD results consist of either the continuous spray of films onto conducting substrates or the spray of isolated droplets onto insulating substrates. A crossover regime, termed here as self-limited electrospray deposition (SLED), has only been limitedly observed in sprays of insulating materials onto conductive substrates. In this case, the rate of film thickness growth continuously declines as the accumulation of charge repels further spray. We examined both the process parameters and material selection to determine the conditions necessary for SLED. Once established, we applied this capability to conformally coat complex three-dimensional objects. Specifically, we noted an opportunity for the post-processing of materials fabricated through additive manufacturing (AM). We employed model substrates to quantitatively study the technique’s limits with regard to geometry and scale. We examined the effectiveness of thickness-limited ESD for coating recessed features with gaps ranging from 50 µm to 1 cm, as well as the ability to coat surfaces hidden from the line-of-sight of the spray needle. This was then extended to the coating of hydrogel lattices printed by AM, demonstrating that coating could be conducted even into the body of the structures as a means to create hydrophobic surfaces, without affecting the absorption-driven humidity response.