Ferumoxytol-enhanced MRI holds potential for the non-invasive assessment of vascular architecture using estimates of cerebral blood volume (CBV). Ferumoxytol specifically enables steady-state imaging with extended acquisition times, for substantial improvements in resolution and contrast-to-noise ratio. With such data, quantitative susceptibility mapping (QSM) can be used to obtain images of local tissue magnetic susceptibility and hence estimate the increase in blood susceptibility after administration of a contrast agent, which in turn can be correlated to tissue CBV. Here, we explore the use of QSM for CBV estimation and compare it with R * (1/T *)-based results. Institutional review board approval was obtained, and all subjects provided written informed consent. For this prospective study, MR images were acquired on a 3.0 T scanner in 19 healthy subjects using a multiple-echo T *-weighted sequence. Scanning was performed before and after the administration of two doses of ferumoxytol (1 mg FE/kg and 4 mg FE/kg). Different QSM approaches were tested on numerical phantom simulations. Results showed that the accuracy of magnetic susceptibility measurements improved with increasing image resolution and decreasing vascular density. In vivo changes in magnetic susceptibility were measured after the administration of ferumoxytol utilizing QSM, and significantly higher QSM-based CBV was measured in gray matter compared with white matter. QSM- and R *-based CBV estimates correlated well, with similar average values, but a larger variance was found in QSM-based estimates.