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In this study, three kinds of electrohydrodynamic atomization (EHDA) processes (electrospraying, electrospinning, and coaxial electrospinning) are implemented to create hydroxypropyl methylcellulose (HPMC) based ultra‐thin products for providing the fast dissolution of a poorly water‐soluble drug ketoprofen (KET). An EHDA apparatus, characterized by a novel spinneret, is homemade for conducting the three processes. The three types of products are electrospun nanofibers E1, electrosprayed microparticles E2, and core‐shell nanofibers E3. SEM and TEM results indicate that they have the anticipated morphologies and inner structures. X‐ray diffraction and Fourier Transform Infrared results verify that KET is mainly amorphous in all the composites due to its fine compatibility with HPMC. In vitro dissolution tests demonstrate that the drug rapid release performances has an order of E3>E1>E2≫KET powders. The fast dissolution mechanisms are suggested and the advantages of the three products are compared. The super performance of E3 in furnishing the rapid release is attributed to a synergistic action of small size (of the shell thickness), high porosity, amorphous state of drug, and the solubility of HPMC. EHDA nanostructures can support the development of nano drug delivery systems (DDSs) through tailoring the spatial distribution of drug molecules within the nano products. [ABSTRACT FROM AUTHOR]