Quantitative susceptibility mapping (QSM) and macromolecular tissue volume (MTV) represent quantitative methods that improve characterization of neurodegenerative diseases. MTV involves acquisition of 3D-Gradient Echo (GRE) at multiple flip angles with long TR and short TE. High-quality QSM requires 3D-GRE at multiple head orientations with long TE. We exploit (i) unused time due to long TR in MTV to collect additional late echoes that allow QSM processing, (ii) acquire each of the multiple flip angles at a different head orientation. These permit simultaneous acquisition of QSM and MTV, whereby two maps are obtained at the scan time of a single contrast.