The effect of isovalent substitution on magnetic function we observe is consistent with previous studies: replacing S with Se in NiPS 3 and Co(NCS) 2 (pyridine) 2 does not produce large changes in the ordering temperature, with a reduction in T c of 5% in NiPS 3 , and an increase in T c of 30% (1.5 K) for Co(NCS) 2 (pyridine) 2 ; 35 but this change does completely switch the single ion anisotropy from easy-plane anisotropy in NiPS 3 to easy-axis anisotropy for NiPSe 3 . The large effects on magnetic properties we observe is in contrast to the layered ZIF analogues where the organic substituents on the imidazolates had relatively small effects on both ordering temperature and fitted superexchange parameters, suggesting that substitution of atoms more directly on the superexchange pathway is critical to produce large effects. Previous work has shown that pressure can tune noncollinearity in MOMs, and so the combination of mechanical and magnetic tunability we demonstrate suggests that doping will be an effective method to modulate strain switchability.