The use of sewage sludge to produce biochar-based sorbents for per- and polyfluoroalkyl substances (PFAS) removal from water and soil may be an economically and environmentally sustainable waste management option. This study compared the sorption of six perfluorinated carboxylic acids (PFCAs) by two sewage sludge biochars (SSBCs) and one wood chip biochar (WCBC), dry pyrolyzed at 700 °C. Batch sorption tests were conducted by adding individual PFCAs and a PFCA-mixture to pure biochars and mixtures of biochar and a sandy soil (1.3% TOC). PFAS-sorption to the SSBCs exhibited log-linear biochar-water distribution coefficients (log K_d), comparable to those previously reported for commercial activated carbons (e.g., 5.73 ± 0.02 for perfluorooctanoic acid at 1 µg/L). The strong sorption of PFCAs was attributed to the SSBCs relatively high pore volumes in the pore size range that can accommodate these compounds. Sorption was attenuated by the presence of soil (by factors 3–10), by the presence of a mixture of PFCAs (by factors of 6–532) and by both together (by factors of 8–6581), indicating strongly competitive sorption between PFCA-congeners, and less severe sorption attenuation by soil organic matter. These findings could enable sustainable value chains for SSBs in soil remediation and water filtration solutions.