By introduction of a new Fe(L1)2 spin-crossover (SCO) unit into the polynuclear system,a nano-scale Fe4(L2)4 molecular square architecture is designed through coordination-directed self-assembly strategy.Both the mononuclear Fe(L1)2 and tetranuclear Fe4(L2)4 complexes have been structurally confirmed by 1H nuclear magnetic resonance (NMR),electrospray ionization time-of-flight mass spectrometry (ESI-TOF-MS),and temperature-dependent single crystal X-ray diffraction studies.Variable-temperature magnetic susceptibility measurements reveal the presence of an abrupt SCO behavior with a thermal hysteresis width of 4 K for Fe(L1)2.By clear contrast,Fe4(L2)4 undergoes a gradual spin transition behavior with enlarged thermal hysteresis width and higher spin transition temperature.