Given the growing popularity of T -weighted/T -weighted (T w/T w) ratio measurements, the objective of the current study was to evaluate the concordance between T w/T w ratios obtained using conventional fast spin echo (FSE) versus combined gradient and spin echo (GRASE) sequences for T w image acquisition, and to compare the resulting T w/T w ratios with histologically validated myelin water fraction (MWF) measurements in several subcortical brain structures. In order to compare these measurements across a relatively wide range of myelin concentrations, whole-brain T w magnetization prepared rapid acquisition gradient echo (MPRAGE), T w FSE and three-dimensional multi-echo GRASE data were acquired from 10 participants with multiple sclerosis at 3 T. Then, after high-dimensional, non-linear warping, region of interest (ROI) analyses were performed to compare T w/T w ratios and MWF estimates (across participants and brain regions) in 11 bilateral white matter (WM) and four bilateral subcortical grey matter (SGM) structures extracted from the JHU_MNI_SS 'Eve' atlas. Although the GRASE sequence systematically underestimated T w/T w values compared to the FSE sequence (revealed by Bland-Altman and mountain plots), linear regressions across participants and ROIs revealed consistently high correlations between the two methods (r = 0.62 for all ROIs, r = 0.62 for WM structures and r = 0.73 for SGM structures). However, correlations between either FSE-based or GRASE-based T w/T w ratios and MWFs were extremely low in WM structures (FSE-based, r = 0.000020; GRASE-based, r = 0.0014), low across all ROIs (FSE-based, r = 0.053; GRASE-based, r = 0.029) and moderate in SGM structures (FSE-based, r = 0.20; GRASE-based, r = 0.17). Overall, our findings indicated a high degree of correlation (but not equivalence) between FSE-based and GRASE-based T w/T w ratios, and low correlations between T w/T w ratios and MWFs. This suggests that the two T w/T w ratio approaches measure similar facets of subcortical tissue microstructure, whereas T w/T w ratios and MWFs appear to be sensitized to different microstructural properties. On this basis, we conclude that multi-echo GRASE sequences can be used in future studies to efficiently elucidate both general (T w/T w ratio) and myelin-specific (MWF) tissue characteristics.