We investigate sodium–calcium silicate glasses implanted with 60 keV Ag+ ions with a dose of 3·1016 cm−2 at an ion current density of 10 μA/cm2. As a result of the ion implantation, a composite layer with silver nanoparticles is synthesized in the region near the surface. However, this layer is characterized by high nonuniformity in the size distribution of these particles over the depth of the layer. Subsequent pulsed laser irradiation in combination with equilibrium heat treatment makes it possible to modify this composite layer, improving the uniformity in the size distribution of the nanoparticles. This is particularly promising for the improvement of the technology of obtaining nonlinear optical materials. To control the parameters of the layers obtained we suggest a method based on an analysis of the optical reflection and transmission spectra measured on the side of the implanted and opposite surfaces of glass samples.