Theoretical and experimental investigations of the particle formation process during spray drying are presented. A novel experimental method allows observation of individual, free flowing droplets during drying in a laminar gas flow and subsequent analysis of the resulting monodisperse, monomorphic dry particles. A second method combines a vibrating orifice generator and a bench top spray drier, which allows production and sampling of monodisperse particles at different drying stages. The experimental results are compared to a full numerical model and a simplified analytical model. Two dimensionless parameters are identified that influence particle formation: the Peclet number, which is the ratio of the diffusion coefficient of the solute and the evaporation rate, and the initial saturation of the excipients. In an application example, particle design is shown to improve the aerosol properties of powders intended for pulmonary drug delivery.