Nano-silica particles decorated with amine groups (S-DA) were prepared via a simple, one-pot method, and under very mild conditions in an attempt to improve the affinity of the silica nanoparticles toward capturing anionic organic dye, namely, methyl orange (MO). The prepared sample was characterized by different techniques such as XRD for crystallinity, SEM for morphological structure, TGA for thermal stability, BET surface area, and FTIR for surface functional groups. The prepared sample was tested for the removal of MO under different conditions including the mass of adsorbent, pH, initial concentration, and time. Results showed that the adsorption of MO was very fast with equilibrium achieved in less than 30 min and a maximum removal efficiency of 100% for a mass to volume ratio of 10 g/3 L, a pH of 2.5, initial concentration of 10 mgL−1, and under stagnant conditions. These results were compared with a bare nano-silica, which was not able to adsorb more than 3% after 24 h, indicating the important effect of amine groups. Furthermore, recycling the adsorbent was achieved by rinsing the MO-loaded adsorbent with a dilute solution of KOH. The adsorbent maintained 50% of its initial removal efficiency after four adsorption–desorption cycles.