What is the source of geogenic (natural or native) solutes in groundwater? The orthodox explanation suggests it is largely a function of water–rock interaction (weathering of the soil zone and aquifer mineral framework). It is proposed herein that atmospheric deposition (combination of wet and dry aerosols from ocean spray, smoke, volcanoes, continental dust, and lightning) is a significant source, and in many cases the dominant source, of the major and minor geogenic solutes in groundwater. Solute mass-balance analyses suggest that much of the mass of major and minor ions must be transported into the aquifer from an external source. Example case studies are presented: analysis of groundwater in a coastal marine aquifer located in an arid area (United Arab Emirates) suggests that over 50% of several major ions potentially originate from atmospheric deposition; in an alluvial fan in a semi-arid system (High Plains, USA), 100% of most solutes potentially originate from atmospheric deposition; and in a humid glacial aquifer system (Michigan, USA), 20–30% of many major ions are potentially from atmospheric deposition. These observations contrast with many hydrogeologic textbooks, which still propose the origin to be water–rock interaction—hence, the myth.