We report the single-crystal growth of Mn2V2O7 and the results of magnetic susceptibility, high-field magnetization up to 55 T and high-frequency electric spin resonance (ESR) measurements for its low-temperature α phase. Two antiferromagnetic (AFM) ordering at 17.5 K and 3 K and obvious magnetic anisotropy are observed in α-Mn2V2O7 upon cooling. In pulsed high magnetic fields, the compound reaches the saturation magnetic moment of ~10.5 μB/f.u. at around 45 T after two undergoing AFM phase transitions at Hc1 ≈ 16 T, Hc2 ≈ 34.5 T for H//[11 ̅0] and Hsf1 = 2.5 T, Hsf2 = 7 T for H//[001]. In these two directions, two and seven resonance modes are detected by ESR spectroscopy, respectively. The ω1 and ω2 modes of H//[11 ̅0] can be well described by two-sublattice AFM resonance mode with two zero-field gaps at 94.51 GHz and 169.28 GHz, indicating a hard-axis feature. The seven modes for H//[001] are partially separated by the critical fields of Hsf1 and Hsf2, displaying the two signs of spin-flop transition. The fittings of ωc1 and ωc2 modes yield zero-field gaps at 69.50 GHz and 84.73 GHz for H//[001], confirming the axis-type anisotropy. The saturated moment and gyromagnetic ratio indicate the Mn2+ ion in α-Mn2V2O7 is in a high spin state with orbital moment completely quenched. A quasi-one-dimensional magnetism with a zig-zag-chain spin configuration is suggested in α-Mn2V2O7, due to the special neighbor interactions caused by a distorted network structure with honeycomb layer.