Conventional phases of matter are described in the limit of thermal equilibrium. Recent advances have suggested that periodically driven, non-equilibrium systems can exhibit novel phases of matter with properties that are highly unusual or not possible in their static counterparts. A broad effort is underway to quantify these systems and explore their applications in quantum information science and materials physics. Hyperpolarized nuclear spin systems have properties that are favorable toward enabling these studies. Conventionally probed by Nuclear Magnetic Resonance (NMR), nuclear spins are highly coherent quantum objects that can be controlled via resonant radiofrequency (RF) pulses. This thesis focuses on $^{13}$C nuclear spins in diamond, which can be hyperpolarized to highly non-thermal spin state populations via interaction with optically pumped Nitrogen Vacancy (NV) defect centers in the lattice. This hyperpolarization provides a vast acceleration in experiment throughput by $\sim10^{10}$ over conventional thermal NMR, enabling highly precise studies of Floquet prethermalization and discrete time crystalline behavior. Further, two novel techniques for nanoscale magnetic resonance imaging are developed with proofs-of-concept shown using hyperpolarized $^{13}$C.