Estuaries regulate carbon cycling along the land-ocean continuum and thus influence carbon export to the ocean, and global carbon budgets. The Elbe Estuary in Germany has been altered by large anthropogenic perturbations, such as widespread heavy metal pollution, minimally treated wastewater before the 1980s, establishment of wastewater treatment plants after the 1990s, and an overall nutrient and pollutant load reduction in the last three decades. Based on an extensive evaluation of key ecosystem variables, and an analysis of the available inorganic and organic carbon records, this study has identified three ecosystem states in recent history: the polluted (1985–1990), transitional (1991–1996), and recovery (1997–2018) states. The polluted state was characterized by very high dissolved inorganic carbon (DIC) and ammonium concentrations, toxic heavy metal levels, dissolved oxygen undersaturation, and low pH. During the transitional state, heavy metal pollution decreased by 〉 50%, and primary production re-established in spring to summer, with weak seasonality in DIC. Since 1997, during the recovery state, DIC seasonality was driven by primary production, and DIC significantly increased by 〉 23 μmol L−1 yr−1 in the mid to lower estuary, indicating that, along with the improvement in water quality the ecosystem state is still changing. Large anthropogenic perturbations can therefore alter estuarine ecosystems (on the order of decades), as well as induce large and complex biogeochemical shifts and significant changes to carbon cycling.