Ni-M (M = Mo, Fe, Co, Mn or Cr) bicomponent catalysts were prepared through the co-impregnation method for upgrading low H2/CO ratio biomass gas into urban gas through partial methanation coupling with water gas shift (WGS). The catalysts were characterized by N2 isothermal adsorption, X-ray diffraction (XRD), H2 temperature programmed reduction (H2-TPR), H2 temperature programmed desorption (H2-TPD), scanning electron microscopy (SEM) and thermogravimetry (TG). The catalytic performances demonstrated that Mn and Cr were superior to the other three elements due to the increased fraction of reducible NiO particles, promoted dispersion of Ni nanoparticles and enhanced H2 chemisorption ability. The comparative study on Mn and Cr showed that Mn was more suitable due to its smaller carbon deposition rate and wider adaptability to various H2/CO and H2O/CO conditions, indicating its better synergy effect with Ni. A nearly 100 h, the lifetime test and start/stop cycle test further implied that 15Ni-3Mn was stable for industrial application.