Although we show that the choice of transition metal is the key factor determining the magnetic character of these frameworks, we also demonstrate that the organic ligand has a key influence over the resulting properties. Substituting pym for btd changes the tilt-angle between MCl 2 chains, altering the tilt angles betwen chains and hence single-ion anisotropy axes, however the increased exchange in pym analogues counteracts this, reducing the overall tilt angle. The increased interlayer separation in btd analogues also reduces the transition magnetic fields. This suggests that the possibilities for chemical control available in MOMs will allow for tuning of spin texture.