A novel molecular assembly of a cobalt–sulfate coordination polymer and melamine is synthesized under acidic conditions. Bar-shaped pink monocrystals as long as 1 mm are found to align along magnetic field lines in the proximity of a strong magnet. Magnetometry shows no hysteresis at temperatures down to 2 K but instead magnetic anisotropy and antiferromagnetic coupling. X-ray diffraction on a single crystal reveals that the cobalt–sulfate chains are along the shortest lattice vector or the crystal’s long axis. The crystal alignment along the magnetic flux can be attributed to single-ion anisotropy that results in longitudinal antiferromagnetic coupling along the chain. Both structurally and magnetically isotropic crystals of metal–organic hybrid materials can be highly useful as elemental components in magneto-optics.