Quantitative MR relaxometry can provide unique subvoxel information about the microscopic tissue compartments that are present in a large imaging voxel. However, unambiguously distinguishing between these tissue compartments continues to be challenging with conventional methods due to the illposedness of the inverse problem. This paper describes a new imaging approach, which we call T 1 Relaxation-T 2 Relaxation Correlation Spectroscopic Imaging (RR-CSI), that uses two-dimensional relaxation encoding combined with spatially-constrained reconstruction to help overcome illposedness. Results are shown with real data, including what we believe to be the first in vivo demonstration of multidimensional relaxation correlation spectroscopic imaging.