Magnetic resonance techniques have proven to be extremely useful in nearly every scientific discipline, from controlling spin dynamics in condensed matter physics to imaging diseased tissue in biomedical engineering. In the first part of my talk, I will discuss my doctoral work implementing a novel spin-control pulse sequence that overcame well-known barriers to high-resolution MRI of solids, dominated by the need for faster imaging, higher resolution, and stronger signal. My results include the highest resolution MRI of phosphorus (P-31) in bone mineral, the first 3D image of P-31 in an organ where the signal comes predominately from phospholipid membranes, and a reconstruction algorithm that speeds up imaging significantly without cost to image quality. In the last part of my talk, I will discuss my plans to continue expanding beyond conventional magnetic resonance techniques to make use of low-field NMR and sensitive atomic magnetometers as detectors.