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A novel zero‐dimensional dinuclear zinc complex, di‐μ‐acetato‐1:2κ4O:O′‐(μ‐2‐acetyl‐6‐{[(Z)‐2‐bromo‐3‐oxoprop‐1‐en‐1‐yl]azanidyl}phenolato‐1κ2O1,O2:2κ3O1,N,O6)(N,N‐dimethylacetamide‐1κO)dizinc(II), [Zn2(C11H8BrNO3)(CH3COO)2(C4H9NO)] or [Zn2(L)(CH3COO)2(DMA)], 1, was synthesized using (Z)‐3‐[(3‐acetyl‐2‐hydroxyphenyl)amino]‐2‐bromoprop‐2‐enal (H2L), which was synthesized from 1‐(3‐amino‐2‐hydroxyphenyl)ethanone and 2‐bromomalonaldehyde. H2L and 1 were characterized by single‐crystal X‐ray diffraction, FT–IR spectroscopy and elemental analysis. Theoretical calculations of the bond orders and excited state of H2L confirmed that there is extensive electron delocalization in the H2L molecules. Single‐crystal X‐ray diffraction shows that the two Zn atoms are pentacoordinated in distorted trigonal bipyramidal configurations in the crystals of 1. The thermogravimetric analysis of 1 shows that the main frame of the complex remains stable to about 190 °C. Powder X‐ray diffraction (PXRD) analysis shows that 1 possesses high purity and acid and alkali resistance. The intermolecular interactions of H2L and 1 were analyzed using Hirshfeld surface analysis and the results indicate that the H...H and O...H interactions of H2L and 1 play a considerable role in stabilizing the self‐assembly process. [ABSTRACT FROM AUTHOR]