PurposeTo develop an MRSI technique capable of mapping downfield proton resonances in the human brain.MethodsA spectral‐spatial excitation and frequency‐selective refocusing scheme, in combination with 2D phase encoding, was developed for mapping of downfield resonances without any perturbation of the water magnetization. An alternative scheme using spectral‐spatial refocusing was also investigated for simultaneous detection of both downfield and upfield resonances. The method was tested in 5 healthy human volunteers.ResultsDownfield metabolite maps with a nominal spatial resolution of 1.5 cm³ were recorded at 3 T in a scan time of 12 minutes. Cramer‐Rao lower bounds for nine different downfield peaks were 20% or less over a single supraventricular slice. Downfield spectral profiles were similar to those in the literature recorded previously using single‐voxel localization methods. The same approach was also used for upfield MRSI, and simultaneous upfield and downfield acquisitions.ConclusionThe developed MRSI pulse sequence was shown to be an efficient way of rapidly mapping downfield resonances in the human brain at 3 T, maximizing sensitivity through the relaxation enhancement effect. Because the MRSI approach is efficient in terms of data collection and can be readily implemented at short TE, somewhat higher spatial resolution can be achieved than has been reported in previous single‐voxel downfield MRS studies. With this approach, nine downfield resonances could be mapped in a single slice for the first time using MRSI at 3 T.