The Curie-Weiss fitting and magnetic ordering temperature show interactions are stronger for NiCl 2 L than FeCl 2 L. The limitations of powder susceptibility measurements mean that we are unable to disentangle the three nearest neighbour Heisenberg interactions J Cl , J L and J vdW ) and spin-orbit derived terms (D, DMI interactions) through fitting robustly. For these layered materials, considering first Heisenberg superexchange only, T c will depend most critically on the strongest two superexchange interactions (≈ J Cl + J L ), and the Curie-Weiss temperature on the mean interaction (≈ J Cl + J L + J vdw ), and so T c and θ are expected to be similar. The single-ion anisotropy will have a complex effect, but typically leads to a reduction in θ and increase in T c , explaining to some extent the observed discrepancies. Comparison with related compounds finds that both magnetic interactions tend to be stronger for Ni in both frameworks with only metal-ligand-metal connectivity and frameworks with only metalchloride-metal connectivity. The expected hiearchy of interactions is that superexchange through the MCl 2 chain is stronger than through the organic linker, which in turn is much stronger than between the layers, i.e. J Cl > J pym ≈ J btd >> J vdW , which we observed in our previous quantitative inelastic neutron scattering investigations of the related CrCl 2 (pym), which we find an order of magnitude separation between interactions. Fitting of magnetic diffuse scattering does confirm this picture for FeCl 2 (btd), with J btd ≈ J Cl /3. Our DFT calculations suggest that the separation is less clear cut for Ni(II) compounds, with J pym ≈ J Cl and J btd ≈ J Cl /2.