Enclosing functional nanoparticles in stable inorganic supports is important for generating ultra-stable catalytic active sites with good performance and material utilization efficiency. Here we describe a simple method to synthesize ultra-thin Ag nanocrystals with dimensions that are defined by the ∼1.4 nm 2D interlayer separating a layered silicate nanostructure. We call the particles "nanoplates" because they are <1.4 nm thick in one direction and their in-plane dimensions are defined by reaction time. The layered silicate is pillared with dialkylurea, which serves both as a reducing agent for the Ag precursor and immobilizes the Ag nanoplates in the interstitial nanospace. The supported Ag nanoplates showed catalytic activity for hydrolysis of NH3BH3 and generation of H2 at room temperature. These supported Ag nanocatalysts had performance much higher than spherical Ag nanoparticles. They, moreover, had performance and stability comparable to costly supported Pt nanoparticles.