Purpose To compare the diagnostic accuracy of gallium 68 (68Ga)-labeled prostate-specific membrane antigen (PSMA)-11 PET/MRI with that of multiparametric MRI in the detection of prostate cancer. Materials and Methods The authors performed a retrospective study of men with biopsy-proven prostate cancer who underwent simultaneous 68Ga-PSMA-11 PET/MRI before radical prostatectomy between December 2015 and June 2017. The reference standard was whole-mount pathologic examination. Readers were blinded to radiologic and pathologic findings. Tumor localization was based on 30 anatomic regions. Region-specific sensitivity and specificity were calculated for PET/MRI and multiparametric MRI by using raw stringent and alternative neighboring approaches. Maximum standardized uptake value (SUVmax) in the tumor and Prostate Imaging Reporting and Data System (PI-RADS) version 2 grade were compared with tumor Gleason score. Generalized estimating equations were used to estimate population-averaged sensitivity and specificity and to determine the association between tumor characteristics and SUVmax or PI-RADS score. Results Thirty-two men (median age, 68 years; interquartile range: 62-71 years) were imaged. The region-specific sensitivities of PET/MRI and multiparametric MRI were 74% (95% confidence interval [CI]: 70%, 77%) and 50% (95% CI: 45%, 0.54%), respectively, with the alternative neighboring approach (P < .001 for both) and 73% (95% CI: 68%, 79%) and 69% (95% CI: 62%, 75%), respectively, with the population-averaged generalized estimating equation (P = .04). Region-specific specificity of PET/MRI was similar to that of multiparametric MRI with the alternative neighboring approach (88% [95% CI: 85%, 91%] vs 90% [95% CI: 87%, 92%], P = .99) and in population-averaged estimates (70% [95% CI: 64%, 76%] vs 70% [95% CI: 64%, 75%], P = .99). SUVmax was associated with a Gleason score of 7 and higher (odds ratio: 1.71 [95% CI: 1.27, 2.31], P < .001). Conclusion The sensitivity of gallium 68-labeled prostate-specific membrane antigen-11 PET/MRI in the detection of prostate cancer is better than that of multiparametric MRI. © RSNA, 2018 See also the editorial by Civelek in this issue.