The new kinetic spray coating technique, vacuum kinetic spray (aerosol deposition), utilizes the pressure gap between powder hopper and coating chamber which is vacuumed. In this study, to investigate the deposition mechanisms present in the vacuum kinetic spray coatings, α-Al2O3 and glass were chosen as the powder and substrate materials, respectively, and these were considered as the reference materials to examine the effect of free surfaces after particle fractures. Based on the finite-element modeling (using an AUTODYN-2D 12.1), single particle impacts were simulated, and the results elucidated the material shape, temperature variation and mass change of particle due to its fracture during impact. The plots of total mass change as a function of particle impact velocity demonstrate the deposition-optimized velocity zone (DOVZ) for successful deposition. Compared to as-received powders, from the transmission electron microscope (TEM) images, the defects such as dislocations of the ball-milled powders might increase the tendency of the powder particles to fracture upon impact. The cross-section images of the coating showed that the particle sizes of the coating were drastically decreased compared to those of initial powders. During coating, fractured particles enlarged the thermodynamically unstable free surface area and have a tendency of formation of bonding.