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• One pot reaction of β -diketone Sm(III) and Tb(III) luminescence compounds. • EIFD, an material sensitizer to luminescence center ions. • Ancillary ligands donors, improving the luminescence lifetime of compounds. EIFD, LnCl 3 ·6H 2 O (Ln = Sm, Tb) and ancillary ligand are developed to synthesize a sequence of six new β -diketone Sm-based and Tb-based compounds modified to enhance the photoluminescence property, namely Sm(EIFD) 3 (H 2 O)·CH 2 Cl 2 (1), Sm(EIFD) 3 (bpy) (2), Sm(EIFD) 3 (phen)·CH 2 Cl 2 (3), Tb(EIFD) 3 (H 2 O)·CH 2 Cl 2 (4) and Tb(EIFD) 3 (bpy) (5), Tb(EIFD) 3 (phen)·CH 2 Cl 2 (6) (EIFD: 1-(1-ethyl-1H-indol-3-yl)-4,4,4-trifluorobutane-1,3‑dione, bpy = 2,2′-bipyridine, phen = 1,10-phenanthroline). The crystal structures of compounds 1 − 6 with the lanthanide(III) ions of seven (1, 4)/eight (2, 3, 5, 6) coordinated configuration are determined by single-crystal X-ray diffraction. Different non-covalent interactions (NCIs) and their% contribution to the compounds structures and their roles in stabilizing the structure are determined by Hirshfeld surface analysis. The photoluminescence properties of compounds 1 − 6 by substituting the solvent H 2 O with bpy and phen contained nitrogen ancillary ligands are then studied experimentally, leading to a rationalization of their central lanthanide(III) ions emission lifetime. [ABSTRACT FROM AUTHOR]