We use measurements of ocean surface dissolved Al, a global Biogeochemical Elemental Cycling (BEC) ocean model, and the global Dust Entrainment and Deposition (DEAD) model to constrain dust deposition to the oceans. Our Al database contains all available measurements with best coverage in the Atlantic. Vertical profiles and seasonal data exist in limited regions. Observations show that surface dissolved Al is distributed similarly to the dust deposition predicted by DEAD and other models. There is an equatorial Atlantic Al maximum that decreases toward higher latitudes. There are high Al concentrations in the Mediterranean Sea and the Arabian Sea and low concentrations in the Pacific and the Southern Ocean. The ocean basins maintain more distinct Al profiles than Fe profiles in the upper ocean, consistent with a weaker biological influence on Al than Fe. The BEC‐predicted surface dissolved Al compares relatively well with observations. The Al distribution reflects the combined effects of Al input from dust and Al removal by particle scavenging and biological uptake by diatoms. Model‐observed biases suggest a southward shift of maximum dust deposition compared to current dust model predictions. DEAD appears to overestimate deposition north of 30°N in the Pacific and to underestimate deposition south of 30°N. Observed Al concentrations and the ocean model–predicted surface Al lifetime provide a semi‐independent method to estimate oceanic dust deposition. This technique indicates that DEAD may overestimate dust deposition to the north equatorial Atlantic but underestimate in other Atlantic regions, the Southern Ocean, and the Arabian Sea. However, spatial variations in aerosol Al solubility may also contribute to the model‐observation mismatch. Our results have implications for all dust‐borne ocean nutrients including Fe and demonstrate the potential of marine geochemical data to constrain atmospheric aerosol deposition fields.