Purpose: To bring metabolic imaging based on multi-NMR toward practical use from the RF hardware perspective.Methods: A highly integrated RF coil is designed for whole-brain MRI and MRS targeted to five nuclear species: H-1, F-19, P-31, Na-23, and C-13. Dipole antennas and closely loaded local receiver loops are combined in this setup.Results: High-quality in vivo scan results of H-1, P-31, Na-23, and C-13 on healthy volunteers have been achieved. For H-1, the transmit efficiency is 77% of a single-tuned commercial head coil (NOVA 8-transmit [Tx]/32-receive [Rx]; NOVA Medical, Wilmington, MA, USA). For P-31, 110% SNR of a dual-tuned close-fit head-birdcage was achieved at the center of the subject, based on MR experiments on a phantom. For P-31, Na-23, and C-13, bench measurements indicate SNR loss of 15%, 27%, and 30% compared with single-tuned conditions. F-19 performance has been proven to be similar to that of H-1 through bench tests and electromagnetic simulations.Conclusion: With this device, H-1-based anatomic images that are expected to meet clinical requirements, as well as high-quality multi-NMR images and spectra, can be acquired within one scan session without hardware replacement or patient repositioning, enabling morphologic and metabolic MRI within acceptable scan time.