It　is　still　a　great　challenge　to　achieve　high　selectivity　of　CH4　in　CO2　electroreduction　reactions　(CO2RR)　because　of　the　similar　reduction　potentials　of　possible　products　and　the　sluggish　kinetics　for　CO2　activation.　Stabilizing　key　reaction　intermediates　by　single　type　of　active　sites　supported　on　porous　conductive　material　is　crucial　to　achieve　high　selectivity　for　single　product　such　as　CH4.　Here,　Cu2O(111)　quantum　dots　with　an　average　size　of　3.5　nm　are　in　situ　synthesized　on　a　porous　conductive　copper-based　metal-organic　framework　(CuHHTP),　exhibiting　high　selectivity　of　73　%　towards　CH4　with　partial　current　density　of　10.8　mA　cm(-2)　at　-1.4　V　vs.　RHE　(reversible　hydrogen　electrode)　in　CO2RR.　Operando　infrared　spectroscopy　and　DFT　calculations　reveal　that　the　key　intermediates　(such　as　*CH2O　and　*OCH3)　involved　in　the　pathway　of　CH4　formation　are　stabilized　by　the　single　active　Cu2O(111)　and　hydrogen　bonding,　thus　generating　CH4　instead　of　CO.