In this paper, we report a facile one-pot synthesis method to prepare well dispersed silver nanoparticles (NPs) supported on α-zirconium phosphate (α-ZrP) single-layer nanosheets. Silver NPs with a narrow size distribution were reduced on α-ZrP single-layer nanosheet surface due to the electrostatic attractions between the positively charged silver cations and the negatively charged α-ZrP nanosheet support. Three reducing agents: glucose, NaBH4, and tri-sodium citrate were used to reduce Ag+. Transmission electron micrographs show that the reduced silver NPs were well dispersed with a diameter of 18.3 ± 4.4 nm, 48.9 ± 13.8 nm, and 3.5 ± 1.0 nm when reduced by glucose, NaBH4, and tri-sodium citrate, respectively. Overall, we present a facile method to synthesize Ag NPs with various dimensions for widespread applications.