This Research Article reports an unusually high efficiency heterogeneous photodegradation of methyl orange (MO) in the presence of Ag nanoparticle-loaded ZnO quasi-nanotube or nanoreactor (A-ZNRs) nanocatalyst grown on FTO substrate. In typical process, photodegradation efficiency of as high as 21.6% per μg per Watts of used catalyst and UV power can be normally obtained within only a 60-min reaction time from this system, which is 10(3) order higher than the reported results. This is equivalent to the turnover frequency of 360 mol mol(-1) h(-1). High-density hexagonal A-ZNRs catalysts were grown directly on FTO substrate via a seed-mediated microwave-assisted hydrolysis growth process utilizing Ag nanoparticle of approximately 3 nm in size as nanoseed and mixture aqueous solution of Zn(NO3)·6H2O, hexamethylenetetramine (HMT), and AgNO3 as the growth solution. A-ZNRs adopts hexagonal cross-section morphology with the inner surface of the reactor characterized by a rough and rugged structure. Transmission electron microscopy imaging shows the Ag nanoparticle grows interstitially in the ZnO nanoreactor structure. The high photocatalytic property of the A-ZNRs is associated with the highly active of inner side's surface of A-ZNRs and the oxidizing effect of Ag nanoparticle. The growth mechanism as well as the mechanism of the enhanced-photocatalytic performance of the A-ZNRs will be discussed.