The possibilities of successive ionic layer deposition technology for synthesizing the Ag nanoclusters and nanolayers were analyzed in present article. It was shown that this technology, based on successive treatments of appropriate substrates in solution of cations and anions, is acceptable for the controllable forming of the Ag nanoparticles at the surface of different substrates. Results related to characterization of the Ag nanoclusters synthesized using Ag(NH3)2NO3 or AgNO3 precursors were discussed. It was found that the concentration and the size of the Ag nanoparticles deposited on a surface of fused quartz, silica gel, and monocrystalline silicon can be controlled by varying composition and pH of the reagent solutions as well as the number of the deposition cycles. It was established that the size of Ag nanoclusters depending on a synthesis conditions may vary from 1–5 nm to 500 nm. Model explained the growth of Ag clusters during successive ionic layer deposition was discussed as well.