In this study, a novel type of tris(2-acyl-1,3-indandione)-aluminum(III) coordination compounds of the general formula [Al(acind) 3 ]H 2 O, where 2-acyl-1,3-indandione (acind), 2-acetyl-1,3-indandione (aind), 2-benzoyl-1,3-indandione (bind), and 4-methyl-2-benzoyl-1,3-indandione (mbind), were synthesized and characterized by elemental analysis (CHN), Fourier transform infrared (FTIR) and nuclear magnetic resonance (1 H NMR) spectroscopies, thermal analysis (TG/DTG and DTA), and optical absorption spectroscopy in the UV-Vis region. These compounds present remarkably high green luminescence in powder and in thin-film forms. However, when these compounds are applied in glass/ITO/β-NPB/spiro-2CBP/[Al(acind) 3 ]/Al and glass/ITO/β-NPB/ [Al(acind) 3 ]/LiF/Al electroluminescent devices, where spiro-2CBP is 2,7-bis(carbazol-9-yl)-9,9spirobifluorene and β-NPB is N,N'-bis(naphthalen-2-yl)-N,N'-bis(phenyl)-benzidine, the emission color tuned from green to red, reflecting a change from the direct charge recombination in the emitting layer of the [Al(acind) 3 ] complexes to an exciplex-based emission in which [Al(acind) 3 ] complexes and spiro 2-CBP acted as acceptor and donor, respectively. These results suggest that [Al(acind) 3 ] complexes have potential applications as molecular light converter materials for fabricating new electroluminescent devices.