We report on a multi-parametric quantitative method based on four 1x1x2mm3 3D multiple-echo gradient-echo acquisitions (GRE), complemented by AFI for B1+ mapping (whole-brain TA=21min). The most notable parameters derived are water content, T1 and T2*, magnetization transfer ratio (MTR), bound proton fraction (fbound) and magnetization exchange rate (kex). Results are reported from seven volunteers, one post-mortem brains and one tumour patient. The use of multiple contrasts for tissue segmentation is illustrated. Correlations between parameters are investigated with the aim of better understanding sources of T1 relaxation. f_bound and k_ex are found to be lower in tumour than in healthy tissue.