Methods of optical dynamic nuclear polarization (DNP) open the door to the replenishable hyperpolarization of nuclear spins, boosting their NMR/MRI signature by orders of magnitude. Nanodiamond powder rich in negatively charged Nitrogen Vacancy (NV -) defect centers has recently emerged as one such promising platform, wherein 13 C nuclei can be hyperpolarized through the optically pumped defects completely at room temperature and at low magnetic fields. Given the compelling possibility of relaying this 13 C polarization to nuclei in external liquids, there is an urgent need for the engineered production of highly "hyperpolarizable" diamond particles. In this paper, we report on a systematic study of various material dimensions affecting optical 13 C hyperpolarization in diamond particles -especially electron irradiation and annealing conditions that drive NVcenter formation. We discover surprisingly that diamond annealing at elevated temperatures close to 1720 • C have remarkable effects on the hyperpolarization levels, enhancing them by upto 36-fold over materials annealed through conventional means. We unravel the intriguing material origins of these gains, and demonstrate they arise from a simultaneous improvement in NVelectron relaxation time and coherence time, as well as the reduction of paramagnetic content, and an increase in 13 C relaxation lifetimes. Overall this points to significant recovery of the diamond lattice from radiation damage as a result of the high-temperature annealing. Our work suggests methods for the guided materials production of fluorescent, 13 C hyperpolarized, nanodiamonds and pathways for their use as multi-modal (optical and MRI) imaging and hyperpolarization agents.