A new route for the synthesis of yttrium disilicate (mainly a-Y 2 Si 2 O 7 ) powders was reported as ethylenediaminetetraacetic acid (EDTA)-citric acid (CA) complexing process. The thermal decomposition, phase composition, and microstructure of sample were characterized by thermogravimetry-differential thermal analyses, X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy, and field emission scanning microscopy, respectively. The EDTA-CA complexation mechanism was further discussed, and the selected condition to get nanocrystalline Y 2 Si 2 O 7 powders was the precursor with pH 9.38 and heat treatment at around 1050°C. The prepared powders were well crystallized with average crystalline size ca. 50 nm.