Unlike higher spin systems, the source of slow magnetic relaxation in S = ½ single molecule magnets is non-intuitive. Herein the magnetic and structural properties of several low spin Ni(III) systems are investigated in attempt to understand why such a system is able to undergo slow magnetic relaxation. Analyses of a bisulphate containing system suggest the presence of a phonon bottleneck effect; however deuteration of the complex removes the characteristic size dependence. This complex, along with others, exemplify the importance of nuclear spin, hydrogen bonding, and crystallite size and guide us towards a better understanding of S = ½ single molecule magnets.