Silver nanoparticles and zinc hydroxide-layered hybrid materials (AgNPs/ZHL) have been successfully developed as efficient catalysts for the reduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) with sodium borohydride. A facile and rapid visible-light assisted green route was used for the deposition of silver nanoparticles (AgNPs) on the external surface of ZHL material. The resulting AgNPs/ZHL hybrids contained AgNPs with spherical morphology and uniform size distribution. Moreover, the AgNPs/ZHL compounds exhibited excellent catalytic performance (the reduction reaction was finished within 4 min) and reusability (three cycles) toward the reduction of 4-NP to 4-AP in presence of sodium borohydride. The reduction reaction obeyed the pseudo-first-order kinetics. The rate constants increased with the increase of amount of the AgNPs deposited into the hybrid materials. These results suggest that the as-prepared catalysts (AgNPs/ZHL) have great potential for heterogeneous catalytic applications.