The major obstacle of methane production from lignocellulose lies in the inefficient deconstruction of biomass. In this study, an anaerobic microbial consortium TC-5 was enriched with high lignocellulose-degradation capacity to enhance methane production from wheat straw. High degradation ratio of 45.7% of un-pretreated wheat straw was achieved due to a multi-species lignocellulolytic enzyme presented in the crude culture supernatant. The specific activity of xylanase, xylan esterase and beta-xylosidase reached the highest level of 4.23, 0.15 and 0.48 U/mg, while cellobiohydrolase, endoglucanase and beta-glucosidase showed the highest specific activity of 0.36, 0.22 and 0.41 U/mg during 9 days' degradation. Inoculation of TC-5 in digestion sludge during anaerobic digestion of wheat straw resulted in remarkable enhancement of 22.2% and 36.6% in methane yield under mesophilic and thermophilic conditions, respectively. This work demonstrates the potential of TC-5 for enhancing the production of biogas and other chemicals through biomass based biorefinery.