We propose a method to enhance lysozyme trapping and supported-Copper catalysis when confined in organosilica materials. The direct synthesis presented here allows the control of the silica surface hydrophobicity by uniform introduction of methyl or phenyl groups. As a result, the lysozyme trapping is observed to be 3.2 times more efficient with the phenyl-functionalized material than MCM-41. For heterogeneous catalysis, Copper was immobilized on the new organosilica surface. In this case, the presence of methyl groups significantly enhanced the product yield for the catalyzed synthesis of a triazole derivative. This method opens a new route of synthesis where the material properties can be adjusted and dedicated to a specific application.