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Electrospray deposition (ESD) uses strong electric fields to produce generations of monodisperse droplets from solutions and dispersions that are driven toward grounded substrates. When soft materials are delivered, the behavior of the growing film depends on the film’s ability to dissipate charge, which is strongly tied to its mobility for dielectric materials. Accordingly, there exist three regimes of electrospray: electrowetting, charged melt, and self-limiting. In the self-limiting regime, it has been recently shown that the targeted nature of these sprays allows for corona-free 3D coating. While ESD patterning on the micron-scale has been studied for decades, most typically through the use of insulating masks, there has been no comparative study of this phenomenon across spray regimes. Here, we used test-patterns composed of gratings that range in both feature size (30–240 μm) and spacing (⅓x–9x) to compare materials across regimes. The sprayed patterns were scanned using a profilometer, and the density, average height, and specificity were extracted. From these results, it was demonstrated that material deposited in the self-limiting regime showed the highest uniformity and specificity on small features as compared to electrowetting and charged melt sprays. Self-limiting electrospray deposition is, therefore, the best suited for modification of prefabricated electrode patterns.