Interstitial patterning of nuclear spins is a nascent design principle for controlling electron spin superposition lifetimes in open-shell complexes and solid-state defects. Herein we report the first test of the impact of the patterning principle on ligand-based nuclear spin dynamics. We test how substitutional patterning of H-1 and Br-79/81 nuclear spins on ligands modulates proton nuclear spin dynamics in the ligand shell of metal complexes. To do so, we studied the H-1 nuclear magnetic resonance relaxation times (T-1 and T-2) of a series of eight polybrominated catechol ligands and six complexes formed by coordination of the ligands to a Ti(IV) ion. These studies reveal that H-1 T-1 values can be enhanced in the individual ligands by a factor of 4 (from 10.8(3) to 43(S) s) as a function of substitution pattern, reaching the maximum value for 3,4,6-tribromocatechol. The T-2 for H-1 is also enhanced by a factor of 4, varying by similar to 14 s across the series. When complexed, the impact of the patterning design strategy on nuclear spin dynamics is amplified and H-1 T-1 and T-2 values vary by over an order of magnitude. Importantly, the general trends observed in the ligands also match those when complexed. Hence, these results demonstrate a new design principle to control H-1 spin dynamics in metal complexes through pattern-based design strategies in the ligand shell.