The impact of surface roughness of bare and zeolite ZSM-5 coated stainless steel and aluminum alloy on colloid deposition has been investigated using a parallel plate flow chamber system in an aqueous environment. The metals were systematically polished to alter the surface roughness from nanoscale to microscale, with the subsequent surface roughness of both the bare and coated surfaces varying from 11.2 to 706 nm. The stainless steel and aluminum alloy surfaces are extensively characterized, both as bare and as coated surfaces. Experimental results suggest that ZSM-5 coating and surface roughness have a pronounced impact on the kinetics of the colloid deposition. The ZSM-5 coating reduced colloid adhesion compared to the corresponding bare metal surface. In general, the greater surface roughness of like samples resulted in higher colloid deposition. Primarily, this is due to greater surface roughness inducing less reduction in the attractive interactions occurring between colloids and collector surfaces. This effect was sensitive to ionic strength and was found to be more pronounced at lower ionic strength conditions. For the most electrostatically unfavorable scenario (ZSM-5 coatings in 1 mM KNO3), the enhanced deposition may also be attributed to inherent surface charge heterogeneity of ZSM-5 coatings due to aluminum in the crystalline structure. The two exceptions are ZSM-5 coated mirror-polished stainless steel and the unpolished aluminum surfaces, which are rougher than the other two samples of the same metal type but result in the least deposition. The reasons for these observations are discussed, as well as the effect of surface charge and hydrophobicity on the adhesion. The relative importance of surface roughness versus contributions of electrostatic interactions and hydrophobicity to the colloid deposition is also discussed.