KCl-extractable sediment dissolved organic nitrogen (KS-DON) extracted from sediments near drinking water intakes of six drinking water sources in Taihu Lake in China was partitioned into hydrophobic and hydrophilic fractions and high/low molecular weight fractions. The results showed that the total dissolved nitrogen (TDN) contents of the extracts ranged from 67.78 to 128.27 mg/kg. KS-DON was the main TDN species, accounting for more than 50%, with NH4+-N and NO3−-N averaging 30% and 20%, respectively. The molecular weight fractions of <1 kDa accounted for almost half of KS-DON. Hydrophilic compounds accounted for more than 75% of KS-DON. Three fluorescence peaks were identified: soluble microbial byproducts (A); protein-like substances (B); and humic acid-like substances (C). It is concluded that the KS-DON in Taihu Lake sources has higher bioavailability and higher risk of endogenous release. Ecological dredging and establishment of constructed wetlands are possible measures to reduce the release of endogenous nitrogen.