Three new heterometallic [CrIII8NiII6] coordination cubes of formulae
[CrIII8NiII6L24(H2O)12](NO3)12 (1), [CrIII8NiII6L24(MeCN)7(H2O)5](ClO4)12 (2) and [CrIII8NiII6L24Cl12] (3) (where
HL = 1-(4-pyridyl)butane-1,3-dione), were synthesised using the paramagnetic metalloligand [CrIIIL3] and
the corresponding NiII salt. The magnetic skeleton of each capsule describes a face-centred cube in which
the eight CrIII and six NiII ions occupy the eight vertices and six faces of the structure, respectively. Direct
current magnetic susceptibility measurements on (1) reveal weak ferromagnetic interactions between the
CrIII and NiII ions, with JCr-Ni = +0.045 cm-1
. EPR spectra are consistent with weak exchange, being dominated
by the zero-field splitting of the CrIII ions. Excluding wheel-like structures, examples of large
heterometallic clusters containing both CrIII and NiII ions are rather rare, and we demonstrate that the use
of metalloligands with predictable bonding modes allows for a modular approach to building families of
related polymetallic complexes. Compounds (1)-(3) join the previously published, structurally related
family of [MIII8MII6] cubes, where MIII = Cr, Fe and MII = Cu, Co, Mn, Pd. <br>