Microbubble–solid surface interaction and attachment under the influence of hydrodynamic and physicochemical forces were studied experimentally and theoretically. An impinging-jet technique was developed to measure bubble-attachment flux onto a flat solid surface in an impinging-jet stagnation flow. A video imaging system enables direct observation of the attachment behavior of hydrogen microbubbles onto two different collector surfaces: hydrophilic untreated glass and hydrophobic methylated glass. Experimental results showed that the attachment flux depends on both hydrodynamic flow and electrolyte concentration. A mass-transfer model developed computes bubble-attachment flux, considering hydrodynamic convection, Brownian diffusion, migration under gravitational buoyancy, and DLVO surface forces (that is, van der Waals and electric double-layer forces). At high flow rates, the numerical predictions for attachment rates onto methylated glass generally agreed well with the experimental data. However, a difference exists between theoretical and experimentally determined attachment rates for both untreated and methylated glass when the Reynolds number of the flow is low. Several mechanisms are proposed to account for this discrepancy.