Rational design of magnetic materials with desired magnetic properties has attracted wide interest in recent decades. Herein, we present a new 2D cobalt(II) metal-organic framework, namely [Co(MQ)_2(V_2O_6)_2]_n·4 nH_2O 1, which was hydrothermally synthesized by the reaction of Co(NO_3)_2·4H_2O, N-methyl-4,4′-bipyridinium (MQ+) chlorine salt and NH_4VO_3. Single-crystal X-ray diffraction analysis reveals that 1 crystallizes in C2/c space group with a = 16.290(5), b = 7.815(2), c = 25.297(7) A, β = 108.459(5)°, V = 3054.8(15) A~3, Z = 4, D_...