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 (