Gradient and spin echo (GRASE) is widely employed in arterial spin labeling (ASL) as an efficient readout sequence. Hemodynamic parameter mappings of perfusion, such as cerebral blood flow (CBF) and arterial transit time (ATT), can be derived via multi-delay ASL acquisitions. Multi-delay ASL perfusion imaging inevitably suffers limited signal-to-noise ratio (SNR) since a motion-sensitized vessel suppressing module has to be employed to highlight perfusion signals. The present work reveals that in multi-delay ASL, manipulation of GRASE sequence on either planar imaging echo echo train for adjusted spatial resolutions or FSE echo train for modulated extent of T2-blurring can significantly alter the mapping contrasts among tissues and among cerebral lobes under different pathways of blood circulation, and meanwhile regulates SNR. Four separate multi-delay ASL scans with different echo train designs in 3D whole brain covering GRASE were carried out for healthy subjects to evaluate the variations in regard to the parameter quantifications and SNR. Based on the quantification mappings, the GRASE acquisition with moderate spatial resolution (3.5 × 3.5 × 4 mm3) and segmented kz scheme was recognized for the first time to be recommended for more unambiguous CBF and ATT contrasts between GM and WM in conjunction with more enhanced ATT contrast between anterior and posterior cerebral circulations, with reasonably good SNR. The technical proposal is of great value for the cutting-edge research of a variety of neurological diseases of global concerns.