Oxides, hydroxides, and other surface films act as impediments to metallurgical bonding during cold spray impact adhesion, raising the critical adhesion velocity and reducing the quality of the deposited coating. Using a single-particle impact imaging approach we study how altering the passivating surface oxides with exposures to various levels of heat and humidity affect the cold spray critical adhesion veloc- ity in the case of aluminum. We analyze the thickness, composition and microstructure of the passivation layers with transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and Fourier- transform infrared spectroscopy (FTIR), and correlate our observations with a direct measurement of the critical adhesion velocity for each surface treatment. We conclude that exposures to temperatures as high as 300 °C for up to 240 min in dry air, or to room-temperature with humidity levels as high as 50% for 4 days, have negligible effect on the surface oxide layers, and by extension do not affect the critical adhesion velocity. In contrast, ambient-temperature exposure to 95% relative humidity levels for 4 days increases the critical adhesion velocity by more than 125 m/s, approximately a 14% percent increase. We observe that this distinct change in critical adhesion velocity is correlated with unique changes in the passivating layer thickness, thickness uniformity, crystallinity and composition resulting from exposure to high humidity. These results speak to particle surface treatments to improve the cold spray process.