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The presence of perfluoroalkyl acids (PFAAs) in biosolids destined for use in agriculture has raised concerns about their potential to enter the terrestrial food chain via bioaccumulation in edible plants. Uptake of PFAAs by greenhouse lettuce (Lactuca sativa) and tomato (Lycopersicon lycopersicum) grown in an industrially impacted biosolids-amended soil, a municipal biosolids-amended soil, and a control soil was measured. Bioaccumulation factors (BAFs) were calculated for the edible portions of both lettuce and tomato. Dry weight concentrations observed in lettuce grown in a soil amended (biosolids:soil dry weight ratio of 1:10) with PFAA industrially contaminated biosolids were up to 266 and 236 ng/g for perfluorobutanoic acid (PFBA) and perfluoropentanoic acid (PFPeA), respectively, and reached 56 and 211 ng/g for PFBA and PFPeA in tomato, respectively. BAFs for many PFAAs were well above unity, with PFBA having the highest BAF in lettuce (56.8) and PFPeA the highest in tomato (17.1). In addition, the BAFs for PFAAs in greenhouse lettuce decreased approximately 0.3 log units per CF2 group. A limited-scale field study was conducted to verify greenhouse findings. The greatest accumulation was seen for PFBA and PFPeA in both field-grown lettuce and tomato; BAFs for PFBA were highest in both crops. PFAA levels measured in lettuce and tomato grown in field soil amended with only a single application of biosolids (at an agronomic rate for nitrogen) were predominantly below the limit of quantitation (LOO). In addition, corn (Zea mays) stover, corn grains, and soil were collected from several full-scale biosolids-amended farm fields. At these fields, all PFAAs were below the LOQ in the corn grains and only trace amounts of PFBA and PFPeA were detected in the corn stover. This study confirms that the bioaccumulation of PFAAs from biosolids-amended soils depends strongly on PFAA concentrations, soil properties, the type of crop, and analyte.