In conclusion, we report two methods for the synthesis of solidsolutions of NiCl 2 (btd) 1 -x (bod) x . We find that there is an approximately linear dependence of the lattice parameters on ligand substitution, with the expected contraction along the M-L-M chain on doping with the smaller bod ligand. The btd ligand is preferentially incorporated into the structure, likely as it is a more electron rich ligand. Investigation of the mechanical properties using high pressure synchrotron X-ray diffraction showed that incorporation of bod stiffens the framework, primarily due to a reduction in interlayer compressibility, as the layers themselves become slightly more compressible. The canted ferromagnetism is retained on doping but doping tunes the hysteresis, producing a significant reduction (up to 60%) in coercive field. These results demonstrate that functionalisation of organic ligands can be a valuable way to tune both the magnetic function and pressureresponsiveness of van der Waals metal-organic magnets. data and powder X-ray diffraction data. E.M. and M.J.C. analysed the bulk magnetic data. E.M., S.L. and S.P.A. measured and analysed the single crystal X-ray diffraction data. J.P.T. measured the electron diffraction data, J.P.T. and M.J.C. analysed the electron diffraction data. M.J.C. wrote the paper with input from all other authors.