The combination of fMRI with electrophysiology, histology, and neurochemistry promises great insights into a level of neural organization that could have never been studied with either technique alone. My talk will focus on (a) spatially resolved fMRI and MRSI (spectroscopic imaging); (b) the study of in vivo connectivity using fMRI and electrical microstimulation, or manganese-enhanced MRI; (c) combined physiology and MRI for examining the electrical activity occurring during increases and decreases of BOLD activation, and (d) molecular imaging based on smart agents. MRSI optimization enabled sufficiently high spectral dispersion and spatiotemporal resolution to obtain isolated glutamate maps in the primate brain. Ongoing research attempts the differentiation of brain structures in the millimeter range and/or detection of small concentration differences in the same structure (activated vs. non-activated cortex). Finally, I will report our first attempt (a) to develop chelates for Gd and endow them with the appropriate coordinating groups that reversibly block some of the Gd’s free coordination sites with changes in pH or [Ca++].