Naturally occurring radon-222 ( 222 Rn) is an effective marker of groundwater inflow to streams, lakes, and coastal environments. However, 222 Rn activity in groundwater is difficult to predict, and existing data are rarely interpreted in a hydrogeologic context. A total of 3582 dissolved 222 Rn samples in groundwater, 302 streamwater samples, and 10 samples from springs across California were used to understand the large-scale patterns of 222 Rn in the state's groundwater. In addition to 222 Rn activity, 54 additional analytes for the same samples together with surficial geology and well depth were used to assess controls on 222 Rn in groundwater. The results show that the lithology of the host formation is the most reliable predictor of 222 Rn activity in groundwater and that 222 Rn activity in groundwater is correlated most strongly with radiological (parent) constituents, further implicating the importance of the host lithology/mineralogy. We created a map of interpolated 222 Rn activity in groundwater across California, which should be a valuable reference for investigations of surface water−groundwater exchanges and potential health effects of 222 Rn in drinking water. The interpolated values from the map provide a rough approximation for experimental planning purposes and for assessing groundwater flux to surface water in areas where groundwater samples are inaccessible.