A novel compound Ni(phen)(H2O)(V2O6) has been hydrothermally synthesized and structurally determined to be a two-dimensional compound, which contains {V2O6}n2n- chains interconnected by nickel(II) complexes via oxygen atoms. The crystallographic data measured by single-crystal X-ray diffraction analysis are as follows: C12H10N2NiO7V2, Mr=454.81, monoclinic, space group P21 / c, a=0.784 6(3), b=2.103 6(8), c=0.942 3(4) nm, β=112.872(5)°, V=1.433 0(10) nm3, Z=4, Dc=2.104 Mg·m-3, μ(Mo Kα)=2.615 mm-1, F(000)=904, T=298(2) K, 4 480 reflections collected, 2 470 independent (Rint=0.032 2), the final R=0.058 4 and wR2=0.145 7 for 2 303 observed reflections with I>2σ(I). CCDC: 192520. A novel compound Ni (phen) (H2O) (V2O6) has been hydrothermally synthesized and structurally determined to be a two-dimensional compound, which contains {V2O6} n2n- chains interconnected by nickel (II) complexes via oxygen atoms. The crystallographic data measured by single-crystal X-ray diffraction analysis are as follows: C12H10N2NiO7V2, Mr = 454.81, monoclinic, space group P21 / c, a = 0.784 6 (3), b = 2.103 6 (8), c = 0.942 3 ), β = 112.872 (5) °, V = 1.433 0 (10) nm3, Z = 4, Dc = 2.104 Mg · m-3 and μ (Mo Kα) = 2.615 mm- , T = 298 (2) K, 4 480 reflections collected, 2 470 independent (Rint = 0.032 2), the final R = 0.058 4 and wR2 = 0.145 7 for 2 303 observed reflections with I> 2σ (I). CCDC: 192520.