Also known as electrospray, electrohydrodynamic atomization has been used extensively in the last 15 years to develop polymer-based particles for drug delivery in cell and animal models. More recently, novel core-shell, multi-axial, and other electrospray particles have been developed from an array of polymers for a variety of biomedical applications. This review focuses on electrospray as a novel method of particle fabrication for drug delivery, specifically highlighting the applications of these particle systems in cell culture and animal models while also discussing polymers used for particle fabrication. Applications of electrospray particles to treat glioma, ovarian cancer, and breast cancer are reviewed. Additionally, delivery of antibiotics, gene therapy, and bacterial cells formulated in electrospray particles is discussed. Finally, vaccines as well as drug eluting particles for differentiation of stem cells and tissue engineering are highlighted. The article concludes with a discussion of where the future of electrospray technology can go to strengthen its foothold in the biomedical field.