A technique is demonstrated to obtain interleaved proton (1H) and 1H-decoupled phosphorus (31P) spectra of human brain using 2D CSI. A modified commercial full-body imager and a dual-tuned birdcage head-coil were employed. Because proton relaxation times are shorter than those of phosphorus, TR(1H) can be chosen to be shorter than TR(31P), thus permitting a 1H acquisition to be inserted in each 31P cycle. The scheme results in significant time savings as both CSI data sets are obtained concurrently with patient loading, coil tuning, shimming, and imaging needed to be done only once.