Aluminum particles were exposed to gaseous polydimethylsiloxane (PDMS) to produce a hydrophobic surface coating for enhanced flow and fluidity. Surface retention of the intact PDMS was confirmed through infrared and X-ray photoelectron spectroscopy. Transmission electron microscopy was used to image cross-sections of the treated particles and energy dispersive spectroscopy element maps demonstrated the presence of a surface layer consisting of silicon and oxygen. Density measurements provided evidence for improvements in the Hausner ratio and Carr index of the PDMS-treated aluminum, indicating a reduction in inter-particulate cohesion through increased bulk density. Stability, compressibility, shear, aeration, and permeability of the particles were assessed by powder rheometer. The compressibility was reduced by approximately 32% following surface treatment, revealing a reduction in void space, while Mohr's circle analysis and shear testing determined that the extrapolated cohesion value was reduced by approximately 53% and the flow factor at 6 kPa was doubled. Aeration testing showed that the air velocity required to obtain a fluidized bed was on the order of 0.35 mm/s for the treated powder, whereas the raw powder could not be uniformly fluidized. PDMS may be a viable option for the large-scale treatment of aluminum powder for flow applications.