Saline-surface crusts and their compositions at ephemeral, dry, and drying lakes are important products of arid-land processes. Detailed understanding is lacking, however, about interactions among locally variable hydrogeologic conditions, compositional control of groundwater on vadose zone and surface salts, and dust composition. Chemical and physical data from groundwater, sediments, and salts reveal compositional controls on saline-surface crusts across a wet playa, Mojave Desert, with bearing on similar settings elsewhere. The compositions of chemically and isotopically distinctive shallow (<3 m) water masses are recorded in the composition of associated salts. In areas with deeper and more saline groundwater, however, not all ions are transported through the vadose zone. Retention of arsenic and other elements in the vadose zone diminishes the concentrations of potentially toxic elements in surface salts, but creates a reservoir of these elements that may be brought to the surface during wetter conditions or by human disturbance. Selective wind-erosion loss of sulfate salts was identified by the compositional contrast between surface salt crusts and underlying groundwater. At the sub-basin scale, compositional links exist among groundwater, salt crusts, and dust from wet playas. Across the study basin, however, lateral variations in groundwater and solid-salt compositions are produced by hydrogeologic heterogeneity.