Hybrid inorganic–organic framework materials exhibit unique properties that can be advantageously tuned through choice of the inorganic and organic components and by control of the crystal structure. We present a new hydrothermally prepared 3D hybrid framework, [Mn(2-methylsuccinate)]n (1), comprising alternating 2D manganese oxide sheets and isolated MnO6 octahedra, pillared via syn, anti–syn carboxylates. Powder magnetic characterization shows that the compound is a homospin MnII ferrimagnet below 2.4 K. The easy-axis is revealed by single-crystal magnetic susceptibility studies and a magnetic structure is proposed. Anisotropic elastic moduli and hardness, observed through nanoindentation on differing crystal facets, were correlated with specific structural features. Such measurements of anisotropy are not commonly undertaken, yet allow for a more comprehensive understanding of structure–property relationships.