Here we evaluate the excess lifetime cancer risk (ELCR) posed by ten PAH-contaminated soils using (i) the currently advocated, targeted chemical-specific approach that assumes dose additivity for carcinogenic PAHs, and (ii) a bioassay-based approach that employs the in vitro mutagenic activity of the soil fractions to determine levels of benzo[a]pyrene equivalents and, by extension, ELCR. Mutagenic activity results are presented in our companion paper (1). The results show that ELCR values for the PAH-containing fractions, determined using the chemical-specific approach, are generally greater (i.e., 8 out of 10) than those calculated using the bioassay-based approach; most are less than 5-fold greater. Only two bioassay-derived ELCR estimates are greater than their corresponding chemical-specific values; differences are less than 10%. The bioassay-based approach, which permits estimation of ELCR without a priori knowledge of mixture composition, proved to be a useful tool to evaluate the chemical-specific approach. The results suggest that ELCR estimates for complex PAH mixtures determined using a targeted, chemical-specific approach are reasonable, albeit conservative. Calculated risk estimates still depend on contentious PEFs and cancer slope factors. Follow-up in vivo mutagenicity assessments will be required to validate the results and their relevance for human health risk assessment of PAH-contaminated soils.