Systems and methods for estimating quantitative parameters of a subject from data acquired using a magnetic resonance imaging (MRI) system. The system includes a computer system configured to control the MRI system to acquire MR fingerprinting (MRF) data representing a plurality of different signal evolutions acquired using different acquisition parameter settings and reconstruct the MRF data into at least one image composed of a plurality of pixels or voxels formed of multiple compartments per pixel or voxel. The computer system is further configured to, on a compartment-by-compartment basis, compare a signal associated with each compartment to an initial dictionary comprising a plurality of signal templates that coarsely sample different acquisition parameters used to acquire the MRF data to determine quantitative parameters for each compartment. The computer system is further configured to generate a quantitative parameter map that indicates the quantitative parameters for each compartment.