Two new isostructural iron(II) complexes 1 and 2, with the formula of Fe(1,4-dcb)(N(CN) 2 ) 2 (1,4-dcb = 1,4-dichlorobenzene), have been prepared and characterized. 1 was obtained under the ambient condition, whereas 2 was prepared by the application of an external magnetic field with a strength of 0.5 T. Single-crystal X-ray structural analysis and Hirshfeld calculations have revealed that the external magnetic fields have induced the disorder of 1,4-dcb molecules in 2, which strengthened the Cl•••N halogen-bonding contacts between 1,4-dcb arrays and one-dimensional (1D) Fe(N(CN) 2 ) 2 chains. As a consequence, coplane stacking of 1,4-dcb arrays and 1D Fe(N(CN) 2 ) 2 chains has been observed in 2. Compared with the stepped stacking and paramagnetic character for 1, the coplane stacking in 2 has increased the lattice cooperativity and ligand-field strength of N(CN) 2 , which thus provided partial spin-state transition. While under 1.0 T, the complex was broken and resulted in the formation of crystals Fe(ClO 4 )•6(H 2 O), suggesting significantly the different influence of magnetic field strength on paramagnetic ions and antimagnetic organic molecules. These results have provided an effective strategy for molecular design with desired physical−chemical properties.