Using a 4.1T whole body system, we have acquired 1H spectroscopic imaging (SI) data of N-acetyl (NA) compounds, creatine (CR), and choline (CH) with nominal voxel sizes of 0.5 cc (1.15 cc after filtering). We have used the SI data to estimate differences in cerebral metabolites of human gray and white matter. To evaluate the origin of an increased CR/NA and CH/NA ratios in gray matter relative to white matter, we measured the T1 and T2 of CR, NA, and CH in gray and white matter using moderate resolution SI imaging. In white matter the T2s of NA, CR, and CH were 233 +/- 27, 141 +/- 18, and 167 +/- 20 ms, respectively, and 227 +/- 27, 140 +/- 16, and 189 +/- 25 ms in gray matter. The T1 values for NA, CR, and CH were 1267 +/- 141, 1487 +/- 146, and 1111 +/- 136 ms in gray matter and 1260 +/- 154, 1429 +/- 233, and 1074 +/- 146 ms in white matter. After correcting for T1 and T2 losses, creatine content was significantly lower in white matter than gray (P < 0.01, t-test), with a white/gray content ratio of 0.8, in agreement with biopsy and in vivo measurements at 1.5 and 2.0T.