We were able to refine the moment directions and magnitudes freely for both iron compounds, but the lower signal-to-noise due to the smaller moment for nickel meant that we had to constrain the moment to lie along the bdirection in NiCl 2 (pym) and NiCl 2 (btd). This meant that we were not directly able to measure the canting, as we were unable to detect any additional peaks that would be a signature of this noncollinearity: a moment along c would produce Bragg intensity for 021 mag. and an a-component would produce intensity at 001 mag. , 020 mag. and 021 mag. peak positions. These refinements produced ordered moments in good agreement with those expected: M 0 = All four compounds have similar magnetic structures, with ferromagnetic correlations along the MCl 2 chains and primarily antiferromagnetic correlations along the b-direction. The interlayer correlations are antiferromagnetic, except for NiCl 2 (btd). In the Ni compounds, the refined moments lie along the bdirection, though the canting is anticipated to occur along the c axis as this is allowed by symmetry. For FeCl 2 (pym) and FeCl 2 (btd) the moments primarily point along the a direction, but cant towards the b axis producing a net intralayer moment in this direction. This net moment is compensated for by the antiferromagnetic alignment with neighbouring vdW layer (Fig. &). A canting angle, γ ND can be determined from the Rietveld refined structures: