Two novel 3D pure inorganic compounds based on [Cr2Py4(mu(4)-O)(2)(mu(3)-OH)(4)](10+) cluster units and sulfate anions are presented. Both complexes exhibit single-molecule-magnet (SMM)-like behavior. Permutation of the magnetic moment direction among SMM-like cluster units has a significant effect on the performance of molecular nanomagnets, and directional consistency shows obvious advantages.