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A novel open-framework vanadium(Ⅳ) phosphate (H3NCH2CH2NH3)3[(VO)4(PO4)2(HPO4)4] (short for V2P3-en) has been prepared. It is synthesized hydrothermally in the presence of ethylenediamine (en) at 170℃ for 5 days by self-assembly from structurally simple precursors V2O5, H3PO4 and H2O. The compound is characterized by means of Fourier transform-infrared spectroscopy (FT-IR), Thermogravimetry-differential thermal analysis (TG-DTA), X-ray powder diffraction analysis (XRD) and Scanning electron microscopy (SEM). Furthermore, the composition-structure-thermal stability relation of V2P3-en is explored in terms of crystal chemistry, and the potential approach to the enhancement of its thermal stability is proposed.