On this research, we efficiently assemble Cu and Si co-doped ultrathin TiO2 nanosheets. As confirmed by complete characterizations, Cu and Si co-doping can rationally tailor the digital construction of TiO2 to maneuver reactive oxygen species for efficient photocatalytic methane conversion. As well as, this co-doping significantly enhances the utilization effectivity of photogenerated expenses. Moreover, it’s revealed that Cu and Si co-doping can considerably increase the adsorption and activation of methane on TiO2 nanosheets. Consequently, the optimized catalyst achieves a C2H6 manufacturing fee of 33.8 µmol g−1 h−1 with a selectivity of 88.4%. This work gives insights into nanocatalyst design towards environment friendly photocatalytic methane conversion into value-added compounds.