Background Although chemical shift-encoded (CSE) MRI proton density fat fraction (PDFF) is the current noninvasive reference standard for liver fat quantification, the liver is more frequently imaged with CT. Purpose To validate quantitative CT measurements of liver fat against the MRI PDFF reference standard. Materials and Methods In this prospective study, 400 healthy participants were recruited between August 2015 and July 2016. Each participant underwent same-day abdominal unenhanced quantitative CT with a calibration phantom and CSE 3.0-T MRI. CSE MRI liver fat measurements were used to calibrate an equation to adjust CT fat measurements and put them on the PDFF measurement scale. CT and PDFF liver fat measurements were plotted as histograms, medians, and interquartile ranges compared; scatterplots and Bland-Altman plots obtained; and Pearson correlation coefficients calculated. Receiver operating characteristic curves including areas under the curve were evaluated for mild (PDFF, 5%) and moderate (PDFF, 14%) steatosis thresholds for both raw and adjusted CT measurements. Sensitivity, specificity, positive predictive value, and negative predictive value were calculated. Results Four hundred volunteers (mean age, 52.6 years ± 15.2; 227 women) were evaluated. MRI PDFF measurements of liver fat ranged between 0% and 28%, with 41.5% (166 of 400) of participants with PDFF greater than 5%. Both raw and adjusted quantitative CT values correlated well with MRI PDFF (r2 = 0.79; P < .001). Bland-Altman analysis of adjusted CT values showed no slope or bias. Both raw and adjusted CT had areas under the receiver operating characteristic curve of 0.87 and 0.99, respectively, to identify participants with mild (PDFF, >5%) and moderate (PDFF, >14%) steatosis, respectively. The sensitivity, specificity, positive predictive value, and negative predictive value for unadjusted CT was 75.9% (126 of 166), 85.0% (199 of 234), 78.3% (126 of 161), and 83.3% (199 of 239), respectively, for PDFF greater than 5%; and 84.8% (28 of 33), 98.4% (361 of 367), 82.4% (28 of 34), and 98.6% (361 of 366), respectively, for PDFF greater than 14%. Results for adjusted CT were mostly identical. Conclusion Quantitative CT liver fat exhibited good correlation and accuracy with proton density fat fraction measured with chemical shift-encoded MRI. © RSNA, 2019 Online supplemental material is available for this article.