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[Display omitted] • MOF-derived porous xPd-NPs@ZIF-8/ZnO were prepared by optimized heat treatment. • Ultrafast high response properties of the sensors were achieved under UV excitation. • Coupling effects of photoexcitation and thermal excitation were explored in detail. • The sensing mechanism of the superior performances were systematically studied. Metal-organic frameworks (MOFs) have been regarded as a potential candidate with great application prospects in the field of gas sensing. Although plenty of previous efforts have been made to improve the sensitivity of MOF-based nanocomposites, it is still a great challenge to realize ultrafast and high selectivity to typical flammable gases in a wide range. Herein, porous xPd-NPs@ZnO were prepared by optimized heat treatment, which maintained the controllable morphology and high specific surface area of 471.08 m2g−1. The coupling effects of photoexcitation and thermal excitation on the gas-sensing properties of nanocomposites were systematically studied. An ultrafast high response of 88.37 % towards 200 ppm H 2 was realized within 1.2 s by 5.0Pd-NPs@ZnO under UV photoexcitation. All xPd-NPs@ZnO exhibited favorable linearity over an extremely wide range (0.2–4000 ppm H 2) of experimental tests, indicating the great potential in quantitative detection. The photoexcited carriers enabled the nanocomposites a considerable response at lower operating temperatures, which made diverse applications of the sensors. The mechanisms of high sensing performances and the photoexcitation enhancement were systematically explained by DFT calculations. This work provides a solid experimental foundation and theoretical basis for the design of controllable porous materials and novel photoexcited gas detection. [ABSTRACT FROM AUTHOR]