Abstract: | Two cadmium(II) and two zinc(II) coordination complexes with diverse structural motifs, [Cd2(HL)I3H2O] · H2O ( 1 ), [Cd2(H2L)2(H2O)4] · 2SO4 · 14H2O ( 2 ), [Zn3(L′)2(H2O)6] · 4H2O · 2(NO3) ( 3 ), and [Zn3L'2(H2O)2Cl2] · H2O ( 4 ) [H2L = 1,1‐bis(5‐(pyrid‐2‐yl)‐1,2,4‐triazol‐3‐yl)methane; H2L′ = 1,1‐bis(5‐(pyrid‐2‐yl)‐1,2,4‐triazol‐3‐yl)methanone] were synthesized through a hydrothermal method. These coordination complexes were characterized by single‐crystal X‐ray diffraction, powder X‐ray diffraction (PXRD), FT‐IR spectroscopy, and photo‐luminescent experiments. Single crystal structural analysis revealed that 1 – 4 belong to polynuclear coordination compounds. PXRD analysis of 1 – 4 unambiguously confirmed the purity of the as‐synthesized coordination compounds. It is the first time to synthesize coordination compounds based on H2L′, which reacted from the original material H2L through in‐situ hydrothermal conditions. In addition, photo‐luminescent experiments revealed that 1 – 4 have real‐time sensing effects for benzaldehyde through fluorescence quenching. For 1 – 4 , the photo‐luminescent quenching effect for benzaldehyde was also compared and the coordination complexes 3 and 4 based on H2L′ have higher photo‐luminescent quenching effect than compounds 1 and 2 . |