Inelastic neutron scattering and high-field electron paramagnetic resonance data are presented for [Mn(bpia)(OAc)-(OCH3)](PF6), where bpia is bis(picolyl) (N-methylimidazole-2-yl)amine. Modeling of the data to the conventional fourth-order spin-Hamiltonian yielded the following parameters: D = 3.526(3) cm(-1), E = 0.588(6) cm(-1), B-4(0) = -0.00084(7) cm(-1), B-4(2) = -0.002(2) cm(-1), B-4(4) = -0.0082(5) cm(-1), g(x) = 1.98(1), g(y) = 1.952(6), and g(z) = 1.978(5). The complex is of particular interest given the biochemical activity and the unusual stereochemistry distinguished by a rare example of a tetragonally compressed octahedron and a pronounced angular distortion imposed by the tetradentate tripodal bpia ligand. Ligand field, density functional theory, and complete active space self-consistent field ab initio calculations are presented that aim to relate the spectroscopic data to the molecular geometry.