This work examines the feasibility of three-dimensional phosphorus-31 magnetic resonance spectroscopic imaging (31P MRSI) of metabolites in the human body using nonselective excitation with a single large circular surface coil for transmitting and receiving. The potential and limitations of this approach to clinical imaging are demonstrated on four selected examples: normal liver and heart, hematoma in the calf, and lymphoma in the groin. The obtained metabolite images showed anatomical detail and allowed differentiation of body organs and pathologic tissue from adjacent tissue. Three-dimensionally localized 31P spectra were reconstructed from nominal volumes of 4 to 15 cm3. These spectra showed characteristic resonances and metabolite intensity ratios for the tissue of origin demonstrating good three-dimensional localization. We conclude that surface coil 31P MRSI of body organs to map metabolite distributions is practically feasible with this approach, but due to experimental limitations, clinical utility requires technical improvements.