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Abstract The laminar combustion characteristics of CH4/air premixed flames with CO2 addition are systemically studied. Experimental measurements and numerical simulations of the laminar burning velocity (LBV) are performed in CH4/CO2/Air flames with various CO2 doping ratio under equivalence ratios of 1.0–1.4. GRI 3.0 mech and Aramco mech are employed for predicting LBV, adiabatic flame temperature (AFT), important intermediate radicals (CH3, H, OH, O) and NO x emissions (NO, NO2, N2O), as well as the sensitivity analysis is also conducted. The detail analysis of experiment and simulation reveals that as the CO2 addition increases from 0% to 40%, the LBVs and AFTs decrease monotonously. Under the same CO2 doping ratio, the LBVs and AFTs increase first and then decrease with the increase of equivalence ratio, and the maximum of LBV is reached at equivalence ratio of 1.05. The mole fraction tendency of important intermediates and NO x with equivalence ratio and CO2 doping ratio are similar to the LBVs and AFTs. Reaction H + O2 ⇔ O + OH is found to be responsible for the promotion of the generation of important intermediates and NO x under the equivalence ratios and CO2 addition through sensitivity analysis. The sensitivity coefficients of elementary reactions that the increasing of CO2 doping ratio promotes or inhibits formation of intermediate radicals and NO x decreases. Graphical abstract