We present a new method for simultaneous mapping of brain function and metabolism. This method provides an unprecedented capability to simultaneously obtain high-resolution metabolic maps (2.4×2.4×3.0 mm3) and brain functional maps (3.0×3.0×2.6 mm3) of the whole brain coverage (230×230×120 mm3) in 8 minutes. The proposed method extends the subspace-based imaging framework of the SPICE technique with a new data acquisition scheme and exploits the complementary information between MRSI and fMRI signals for high-quality image reconstruction. Brain imaging experiments have been carried out, demonstrating the impressive capability of our method. With further improvement, the method can provide an unprecedented tool for mapping brain function and metabolism simultaneously.