Oxalate-bridged mixed metal assemblies A[Mn(II)Fe(III)(ox)(3)] with large templating cations, A(+) = P(C6H5)(4)(+) and AS(C6H5)(4)(+), exhibited a spin direction almost perpendicular to the honeycomb layers consisting of the alternate array of Mn(II) and Fe(III) ions through oxalate ligands. On the other hand, the spins were aligned parallel to the basal layers in the compound with the small cation, NPr4+. A variation of ca. 70degrees in spin direction was observed for mixed crystals NPr4[Mn(II)Fe(III)(x)Cr(III)(1-x)(ox)(3)].