Methane/methanol conversion is one of the most important chemicalr eactions. Methane monooxygenases from methanotrophs are enzymes that catalyzem ethane/methanol conversion under mild conditions. Here we report the reconstitution of purified photosystem II (PSII) from Thermosynechococcus elongatus BP-1 into the membrane fraction containing particulate methane monooxygenase (pMMO) from Methylosinus trichosporium OB3b. Photoinduced hydroxylation of methane to methanol was successfully achieved by using the PSII-reconstituted membrane containing pMMO under light irradiation. This result indicates that the sequential redox chain from PSII through the quinone pool to pMMO can be constructed and that water can serve as the electron donor for methaneh ydroxylation under irradiation with light. pMMO in the membrane fraction produced hydrogen peroxide as ab yproduct when an electron donor was added for methane hydroxylation, whereas under light irradiation conditions the PSII-reconstituted membrane containing pMMO did not generate hydrogen peroxide. Optimization of the electron-transfer rate can easily be achieved with this systembyt uning the light intensity.Methanei st he dominantc omponent of natural gas, which is a promisinga lternative fuel source because the "shale gas revolution" has led to major increases in viable reserves of natural gas. Methane is also ar enewable form of energy because it can be recycled from carbon dioxide, the full oxidation product of methane, through several enzymaticr eactions. [1,2] Methanei su sually liquefied fore ase of storage or transport; this requires the gas to be cooled to À162 8C. Liquefaction of natural gas accounts for about half of its total cost, with shipping and regasification each accounting for2 5% of the overall cost. Therefore, the conversion of natural gas into al iquid product, referred to as gas-to-liquid (GTL) technology,h as been studied. [3] In particular, the conversion of methanei nto methanol is desirablef or the usage of natural gas. Selective oxidation of methane to methanoli se xtremely difficult chemistry,h owever,b ecause the CÀHb ond in methane has one of the highest bond energies (104 kcal mol À1 )o fa ll organic substrates. Recently,s everal research groups have reported the direct oxidation of methane to methanolb yu sing transitionmetal catalysts, but the development of efficient catalysts for direct conversion of methane into methanol is still one of the most challenging subjects in catalytic chemistry. [4][5][6][7] In nature,m ethanotrophs-bacteria capable of using methane as their sole carbon source-can be employed as biological catalysts for methane hydroxylation. Methane-hydroxylating systemsu sing methanotrophs have been reported previously. [8][9][10] The methane hydroxylationi sc atalyzed by an important class of enzymes known as methane monooxygenases (MMOs) from methanotrophs, which are unique in their capability to mediate the facile conversion of methane into methanolu nder ambient conditions. [11][12][13] Hydroxylation of methane to met...