We report here the syntheses, crystal structures, bulk magnetic properties and magnetic ground states of four vdW layered MOMs: FeCl 2 (pym), FeCl 2 (btd), NiCl 2 (pym) and NiCl 2 (btd). We show they all have noncollinear ground states with large canting and net magnetic moments within each layers, and that three of these materials have significant remnant magnetisation. We use density-functional calculations together with consideration of model Hamiltonians to rationalise the magnetic properties of these materials, providing a framework for the design of new noncollinear vdW MOMs.