A three-coil continuous arterial-spin-labeling technique with a separate neck labeling coil was implemented on a Siemens 3T Trio for quantitative cerebral blood flow (CBF) and CBF fMRI measurements in non-human primates (rhesus monkeys). The optimal labeling power was 2 W, labeling efficiency was 92±2%, and optimal post-labeling delay was 0.8 s. Gray matter (GM) and white matter (WM) were segmented based onT1 maps. Quantitative CBF were obtained in 3 min with 1.5-mm isotropic resolution. Whole-brain average ΔS/Swas 1.0–1.5%. GM CBF was 104±3 ml/100 g/min (n=6, SD) and WM CBF was 45±6 ml/100 g/min in isoflurane-anesthetized rhesus monkeys, with the CBF GM/WM ratio of 2.3±0.2. Combined CBF and BOLD (blood-oxygenation-level-dependent) fMRI associated with hypercapnia and hyperoxia were made with 8-s temporal resolution. CBF fMRI responses to 5% CO2 were 59±10% (GM) and 37±4% (WM); BOLD fMRI responses were 2.0±0.4% (GM) and 1.2±0.4% (WM). CBF fMRI responses to 100% O2 were −9.4±2% (GM) and −3.9±2.6% (WM); BOLD responses were 2.4±0.7% (GM) and 0.8±0.2% (WM). The use of a separate neck coil for spin labeling significantly increased CBF signal-to-noise ratio and the use of small receive-only surface coil significantly increased signal-to-noise ratio and spatial resolution. This study sets the stage for quantitative perfusion imaging and CBF fMRI for neurological diseases in anesthetized and awake monkeys.