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Understanding the methane adsorption mechanism is critical for studying shale gas storage and transport in shale nanopores. In this work, we conducted low-pressure nitrogen adsorption (LPNA), scanning electron microscopy (SEM), and high-pressure methane adsorption experiments on seven shale samples from the Longmaxi formation in Sichuan basin. LPNA and SEM results show that pores in the shale samples are mainly nanometer-sized and have a broad size distribution. We have also shown that methane should be not only adsorbed in micropores (< 2 nm) but also in mesopores (2-50 nm) by two hypotheses. Therefore, we established a novel DA-LF model by combining the micropore filling and monolayer coverage theories to describe the methane adsorption process in shale. This new model can fit the high-pressure isotherms quite well, and the fitting error of this new model is slightly smaller than the commonly used D-A and L-F models. The absolute adsorption isotherms and the capacities for micropores and mesopores can be calculated using this new model separately, showing that 77% to 97% of methane molecules are adsorbed in micropores. In addition, we conclude that the methane adsorption mechanism in shale is: the majority of methane molecules are filled in micropores, and the remainder are monolayer-adsorbed in mesopores. It is anticipated that our results provide a more accurate explanation of the shale gas adsorption mechanism in shale formations. Cited as :  Zhou, S., Ning, Y., Wang, H., Liu, H., Xue, H. Investigation of methane adsorption mechanism on Longmaxi shale by combining the micropore filling and monolayer coverage theories. Advances in Geo-Energy Research, 2018, 2(3): 269-281, doi: 10.26804/ager.2018.03.05.