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To develop a free-breathing multidelay pseudocontinuous arterial spin labeling (pCASL) technique for quantitative measurement of liver perfusion of the hepatic artery and portal vein, respectively.A navigator-gated pCASL sequence with balanced steady-state free precession (bSSFP) readout was developed and applied on five healthy young volunteers at 3T. Two labeling schemes were performed with the labeling plane applied on the descending aorta above the liver, and perpendicular to the portal vein before its entry to liver to label the hepatic artery and portal vein, respectively. For each labeling scheme, pCASL scans were performed at five or six postlabeling delays between 200 and 2000 msec or 2500 msec with an interval of 400 or 500 msec. Multidelay pCASL images were processed offline with nonrigid motion correction, outlier removal, and fitted for estimation of liver perfusion and transit time.Estimated liver perfusion of the hepatic artery and hepatic portal vein were 21.8 ± 1.9 and 95.1 ± 8.9 mL/100g/min, with the corresponding transit time of 1227.3 ± 355.5 and 667.2 ± 85.0 msec, respectively. The estimated liver perfusion and transit time without motion correction were less reliable with greater residual variance compared to those processed with motion correction (P < 0.05).The liver perfusion measurement using multidelay pCASL showed good correspondence with values noted in the literature. The capability to noninvasively and selectively label the hepatic artery and portal vein is a unique strength of pCASL as compared to other liver perfusion imaging techniques, such as computed tomography perfusion and dynamic contrast-enhanced MRI. J. Magn. Reson. Imaging 2016;43:1046–1054.