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The development of new styrene-based hyper-crosslinked nanocomposites (HCLN) containing mesoporous silica nanoparticles (MSN) is reported here as a new strategy to obtain functional high surface area materials with an enhanced hydrophilic character. The HCLN composition, morphology and porous structure were analyzed using a multi-technique approach. The HCLN displayed a high surface area (above 1600 m2/g) and higher microporosity than the corresponding hyper-crosslinked neat resin. The enhanced adsorption properties of the HCLN towards polar organic dyes was demonstrated through the adsorption of a reactive dye, Remazol Brilliant Blue R (RB). In particular, the HCLN containing 5phr MSN showed the highest adsorption capacity of RB.