The goal of this study was to compare the spectral quality and metabolite concentrations obtained with short echo-time 2D spiral MRSI and single-voxel spectroscopy (SVS) in the human brain at 3T. Semi-LASER was used for localization (SVS) or pre-localization (MRSI). MRSI was acquired in a transverse slice through the posterior cingulate cortex (PCC), and SVS was from PCC. Results show comparable spectral quality between acquisitions. Differences in concentrations between the two techniques is likely due to the MRSI point-spread function. This study shows feasibility of acquiring high-quality spiral MRSI data similar in spectral quality to SVS within a few minutes.