Using liquid chromatography tandem mass spectrometry, we determined the first nationwide inventories of 13 perfluoroalkyl substances (PFASs) in U.S. biosolids via analysis of samples collected by the U.S. Environmental Protection Agency in the 2001 National Sewage Sludge Survey. Perfluorooctane sulfonate [PFOS; 403 +/- 127 ng/g dry weight (dw)] was the most abundant PFAS detected in biosolids composites representing 32 U.S. states and the District of Columbia, followed by perfluorooctanoate [PFOA; 34 +/- 22 ng/g dw] and perfluorodecanoate [PFDA; 26 +/- 20 ng/g dw]. Mean concentrations in U.S. biosolids of the remaining ten PFASs ranged between 2 and 21 ng/g dw. Interestingly, concentrations of PFOS determined here in biosolids collected prior to the phase-out period (2002) were similar to levels reported in the literature for recent years. The mean load of Sigma PFASs in U.S. biosolids was estimated at 2749-3450 kg/year, of which about 1375-2070 kg is applied on agricultural land and 467-587 kg goes to landfills as an alternative disposal route. This study informs the risk assessment of PFASs by furnishing national inventories of PFASs occurrence and environmental release via biosolids application on land. (c) 2013 Elsevier B.V. All rights reserved.