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Ag pillared interlayered clays (Ag-PILCs) were synthesized through a novel method, in which Ag nanoparticles were formed in montmorillonite interlayers. In this method, silver ions were first exchanged into montmorillonite interlayers, and then reduced into Ag nanoparticles by trisodium citrate at 100°C in aqueous solutions. The synthesized Ag@montmorillonite nanocomposite was characterized by X-ray diffraction (XRD) and transmission electron microscopy (TEM), and its surface area was evaluated by using Brunauer–Emmet–Teller (BET) method. Compared to traditional PILCs synthesized through ion exchange method, the formed Ag-PILCs had better thermal stability and stronger structure because their pillars are nanoparticles. Furthermore, this method introduces a possibility to control the size of the pillars and thus the pore size of the PILCs, due to that the nanoparticle pillars can be modified on their forms and diameters in the synthesizing process. Also, it was found that the intercalating Ag nanoparticle pillars were formed at restricted pH values and silver ion concentrations.