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Two new phenoxo-bridged heterobimetallic [Zn(II)2M(II)] (M = Sr and Ba) salamo-based complexes, [{Zn(L)(μ2-OAc)}2Sr]·0.33CH3OH·H2O (1) and [{Zn(L)(μ2-OAc)}2Ba] (2), have been designed, self-assembled and characterized by elemental analysis, FT-IR and UV-Vis spectroscopy, X-ray crystallography, Hirshfeld surfaces analyses, and Density Functional Theory (DFT) calculations. The results of UV and fluorescence titration experiments have demonstrated that the coordination ratio of the ligand H2L to Zn(II) has been 1 : 2 in the L–Zn(II) precursor. However, X-ray crystallographic analysis indicates the coordination ratio of H2L to Zn(II) as 1 : 1 in the complexes 1 and 2. Coordination environments of the complexes 1 and 2 are almost similar. The complex 1 has an asymmetric heterotrinuclear structure, while the complex 2 is formed as the symmetric heterotrinuclear structure. Fluorescence spectra demonstrate that fluorescence of the ligand is almost completely quenched due to coordination of Zn(II) atoms with H2L. According to DFT calculations chemical stability of the complexes 1 and 2 is higher than that of H2L. [ABSTRACT FROM AUTHOR]