Surface modification of nanomaterials with polymers is an effective route to render new functions and improve the performance of the final nanocomposites. Here, a facile method was developed to fabricate polyacrylic acid (PAA)-grafted monodisperse SiO2 nanoparticles (SiO2-PDA-PAA) through a combination of mussel inspired chemistry and Michael addition reaction. To obtain the products, the SiO2 nanoparticles were first coated with polydopamine (PDA) through self-polymerization of dopamine under rather mild conditions. The PDA thin films can then be further conjugated with amino-terminated PAA, which was synthesized by chain transfer free radical polymerization using cysteamine hydrochloride as a chain transfer agent and acrylic acid as a monomer. The SiO2-PDA-PAA nanocomposites were characterized via transmission electron microscopy, Fourier transform infrared spectroscopy, thermal gravimetric analysis, and X-ray photoelectron spectroscopy. The effects of contact time, solution pH, temperature and methylene blue (MB) concentration on the removal of MB were investigated. The results demonstrated that SiO2-PDA-PAA showed significant improvement in adsorption efficiency towards MB. The kinetics and isotherm studies showed that pseudo-second-order and Langmuir isotherm models were well fitted the experimental data. The values of thermodynamics parameters such as entropy change (ΔS0), enthalpy change (ΔH0) and Gibbs free energy (ΔG0) were calculated based on the Van’t Hoff equation. The negative values of thermodynamic parameters indicated that the adsorption of MB was a feasible, spontaneous and exothermic process. In summary, we developed a facile method to fabricate SiO2-based polymer nanocomposites, which showed obviously enhanced adsorption capability towards MB.