The racemic conglomerate (1P-NH3 + 1M-NH3) and enantioenriched bulk samples (1P-H2O or 1M-NH3) of Co(II) metal–organic frameworks were obtained from achiral precursors under different solvothermal conditions. The bulk homochirality was generated through asymmetrical crystallization in the absence of any chiral additives confirmed by single crystal X-ray diffraction and CD spectroscopy.