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Solar-driven CO2-to-fuel conversion assisted by another major greenhouse gas CH4 is promising to concurrently tackle energy shortage and global warming problems. However, current techniques still suffer from drawbacks of low efficiency, poor stability, and low selectivity. Here, a novel nanocomposite composed of interconnected Ni/MgAlOx nanoflakes grown on SiO2 particles with excellent spatial confinement of active sites is proposed for direct solar-driven CO2-to-fuel conversion. An ultrahigh light-to-fuel efficiency up to 35.7%, high production rates of H2 (136.6 mmol min-1 g-1) and CO (148.2 mmol min-1 g-1), excellent selectivity (H2/CO ratio of 0.92), and good stability are reported simultaneously. These outstanding performances are attributed to strong metalsupport interactions, improved CO2 absorption and activation, and decreased apparent activation energy under direct light illumination. MgAlOx @SiO2 support helps to lower the activation energy of CH* oxidation to CHO* and improve the dissociation of CH4 to CH3 * as confirmed by DFT calculations. Moreover, the lattice oxygen of MgAlOx participates in the reaction and contributes to the removal of carbon deposition. This work provides promising routes for the conversion of greenhouse gasses into industrially valuable syngas with high efficiency, high selectivity, and benign sustainability. [ABSTRACT FROM AUTHOR]