Polarized neutron diffraction (PND) investigations were conducted for a single-crystal of a dinuclear octahedral high-spin cobalt(II) complex, using the local site susceptibility tensor method. The local induced magnetic moments were observed on cobalt(II) ions, revealing an angle of 37(1)°. Previously the compound was found to show a characteristic magnetic behavior, which was thought to be due to the significant magnetic anisotropy caused by an angle between the local axes of cobalt(II) ions. The angle obtained by PND was in good agreement with the result of magnetic analysis, and PND methods were shown to be very useful for studying highly-anisotropic molecular paramagnetic compounds.