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Color-controlled spherical Ag nanoparticles (NPs) and nanorods, with features that originate from their particle sizes and morphologies, can be synthesized within the mesoporous structure of SBA-15 by the rapid and uniform microwave (MW)-assisted alcohol reduction method in the absence or presence of surface-modifying organic ligands. The obtained several Ag catalysts exhibit different catalytic activities in the H2 production from ammonia borane (NH3BH3, AB) under dark conditions, and higher catalytic activity is observed by smaller yellow Ag NPs in spherical form. The catalytic activities are specifically enhanced under the light irradiation for all Ag catalysts. In particular, under light irradiation, the blue Ag nanorod shows a maximum enhancement of more than twice that observed in the dark. It should be noted that the order of increasing catalytic performance is in close agreement with the order of absorption intensity owing to the Ag localized surface plasmon resonance (LSPR) at irradiation light wavelength. Upon consideration of infrared thermal effect, wavelength dependence on catalytic activity, and effect of radical scavengers, it can be concluded that the dehydrogenation of AB is promoted by change of charge density of the Ag NP surface derived from LSPR. The LSPR-enhanced catalytic activity can be further realized in the tandem reaction consisting of dehydrogenation of AB and hydrogenation of 4-nitrophenol, in which a similar tendency in the enhancement of catalytic activity is observed. [ABSTRACT FROM AUTHOR]