The consequences of groundwater contamination can remain long after a contaminant source has been removed. Documentation of natural aquifer recoveries and empirical tools to predict recovery time frames and associated geochemical changes are generally lacking. This study characterized the long-term natural attenuation of a groundwater contaminant plume in a sand and gravel aquifer on Cape Cod, Massachusetts, after the removal of the treated-wastewater source. Although concentrations of dissolved organic carbon (DOC) and other soluble constituents have decreased substantially in the 15 years since the source was removed, the core of the plume remains anoxic and has sharp redox gradients and elevated concentrations of nitrate and ammonium. Aquifer sediment was collected from near the former disposal site at several points in time and space along a 0.5-km-long transect extending downgradient from the disposal site and analyses of the sediment was correlated with changes in plume composition. Total sediment carbon content was generally low (< 8 to 55.8 μmol (g dry wt)− 1) but was positively correlated with oxygen consumption rates in laboratory incubations, which ranged from 11.6 to 44.7 nmol (g dry wt)− 1 day− 1. Total water extractable organic carbon was < 10–50% of the total carbon content but was the most biodegradable portion of the carbon pool. Carbon/nitrogen (C/N) ratios in the extracts increased more than 10-fold with time, suggesting that organic carbon degradation and oxygen consumption could become N-limited as the sorbed C and dissolved inorganic nitrogen (DIN) pools produced by the degradation separate with time by differential transport. A 1-D model using total degradable organic carbon values was constructed to simulate oxygen consumption and transport and calibrated by using observed temporal changes in oxygen concentrations at selected wells. The simulated travel velocity of the oxygen gradient was 5–13% of the groundwater velocity. This suggests that the total sorbed carbon pool is large relative to the rate of oxygen entrainment and will be impacting groundwater geochemistry for many decades. This has implications for long-term oxidation of reduced constituents, such as ammonium, that are being transported downgradient away from the infiltration beds toward surface and coastal discharge zones.