The distribution of alkyltrimethylammonium compounds (ATMAC), cationic surfactants used in a wide variety of applications, has been determined in sediments from Jamaica Bay (NY). Total concentrations in surficial sediments collected between 1998 and 2008 ranged from 361 to 6750 ng/g. The highest values were found in samples from a deeper basin directly affected by treated wastewater discharges. Behentrimonium, a mixture dominated by a homologue having 22 carbon atoms in its alkyl chain (ATMAC 22), was identified for the first time using time-of-flight mass spectrometry and accounted for approximately 80% of the total ATMAC in recent sediment samples. Analyses of a dated sediment core and subsequent surface grab samples revealed an exponential increase in concentration over the last three decades with a doubling time of 3.9 years. Similar temporal trends were seen in surface samples from other sites in Jamaica Bay and Newton Creek (NY), another site greatly influenced by wastewater discharges. This dramatic increase in ATMAC 22 reflects greater use of behentrimonium and likely replacement of other products containing other ATMAC homologues in personal care products. Further monitoring is recommended to assess the environmental risk and fate of this persistent emerging contaminant.