• 𝑠𝑠 ⃗ � 𝑖𝑖 formalism). There is also no agreement on the sign and magnitude of the zero-field splitting (DNi) for the central or ring Ni II ions. In order to investigate the magneto-structural relationship in this family of complexes further, and to unequivocally extract the relevant spin-Hamiltonian parameters, we have synthesised and characterised the complex [Ni7(hmp)7.55(pic)4.45](ClO4)2•6MeOH (1•6MeOH; Figure , hmpH = 2-(hydroxymethyl)pyridine, picH = picolinic acid) using a combination of susceptibility and magnetisation measurements, magnetic neutron spectroscopy and first principles calculations. This complementary trio of techniques, employed for the first time in the analysis of [Ni7] Anderson wheels, reveals the presence of competing ferro-and antiferromagnetic exchange interactions and both easy plane and easy axis anisotropy.