The distribution of natural organic carbon was investigated at a chloroethene-contaminated site where complete reductive dechlorination of tetrachloroethene (PCE) to vinyl chloride and ethene was observed. In this study, operationally defined potentially bioavailable organic carbon (PBOC) was measured in surficial aquifer sediment samples collected at varying depths and locations in the vicinity of a dense nonaqueous phase liquid (DNAPL) source and aqueous phase plume. The relationship between chloroethene concentrations and PBOC levels was examined by comparing differences in extractable organic carbon in aquifer sediments with minimal chloroethene exposure relative to samples collected in the source zone. Using performance-monitoring data, direct correlations with PBOC were also developed with chloroethene concentrations in groundwater. Results show a logarithm-normal distribution for PBOC in aquifer sediments with a mean concentration of 187  mg/kg. PBOC levels in sediments obtained from the underlying confining unit were generally greater when compared to sediments collected in the sandy surficial aquifer. Results demonstrated a statistically significant inverse correlation (p=0.007) between PBOC levels in aquifer sediments and chloroethene concentrations for selected monitoring wells in which chloroethene exposure was the highest. Results from laboratory exposure assays also demonstrated that sediment samples exhibited a reduction in PBOC levels of 35% and 73%, respectively, after a 72-h exposure period to PCE (20,000  μg/L). These results support the notion that PBOC depletion in sediments may be expected in chloroethene-contaminated aquifers, which has potential implications for the long-term sustainability of monitored natural attenuation.