In this work, we presented the synthesis and characterization of poly-melamine-formaldehyde-silica (PMF‑Si) composite from poly-melamine-formaldehyde (PMF) and previously purified commercial sodium silicate used as a precursor of silica nanoparticles (Si‑NPs). The materials were characterized by several physicochemical techniques such as XRD, FTIR, SEM, TEM, AFM, TGA, and DTG analysis to access their properties. We also studied hydrogel dehydration, rehydration, the potential of zero charge (PZC), and the adsorption capacity of the dye methylene blue (MB) in the hydrogel. From XRD analysis, PMF and PMF‑Si materials presented amorphous profiles. AFM, SEM, and TEM images revealed a fibrous PMF structure and homogeneous dispersion of Si-NPs through the PMF-Si composite. The Si‑NPs exhibited an average diameter between 10 to 15 nm. The first PMF-Si hydration reached 93% after synthesis, and complete rehydration is possible up to 70% of dehydration. PMF-Si has the PZC at pH = 1.22 and, at superior values of pH, the composite exhibits superior adsorption rates of MB. The adsorption tests performed to remove MB dye using PMF-Si hydrogel showed a qmax of 140 mg/g, which is superior to other materials routinely used for MB dye removal.