Simultaneous CO2removal with renewable biofuel production can be achieved by methanogens through conversion of CO2and H2into CH4. However, the low gas-liquid mass transfer (<I>k</I>L<I>a</I>) of H2limits the commercial application of this bioconversion. This study tested and compared the gas-liquid mass transfer of H2by using two stirred tank reactors (STRs) equipped with a micro-nano sparger (MNS) and common micro sparger (CMS), respectively. MNS was found to display superiority to CMS in methane production with the maximum methane evolution rate (MER) of 171.40 mmol/LR/d and 136.10 mmol/LR/d, along with a specific biomass growth rate of 0.15 d<SUP>−1</SUP>and 0.09 d<SUP>−1</SUP>, respectively. Energy analysis indicated that the energy-productivity ratio for MNS was higher than that for CMS. This work suggests that MNS can be used as an applicable resolution to the limited<I>k</I>L<I>a</I>of H2and thus enhance the bioconversion of H2and CO2to CH4..