Understanding the near-surface environment where atmospheric and solid earth processes interact, often termed the “Critical Zone,” is important for assessing resources and building resilient societies. Here, we examine a volcanic landscape in the Oregon Cascade Range, an understudied Critical Zone setting that is host to major regional water resources, pervasive silicate weathering, and significant geohazards. We leverage a bedrock age chronosequence to show that the volcanic Critical Zone undergoes a structural shift, from depth extents of >1 km to meters, over timescales of 1 My. We map an active groundwater volume comparable to major continental lakes, stored at the Cascade Range crest. This state shift makes volcanic landscape evolution a unique probe of deep coupling between Earth systems.