An organic-inorganic hybrid adsorbent was prepared and its application for the uptake of Cu II ions from aqueous solutions was studied. The polymer network was composed of poly(dimethylsiloxane) (PDMS), vinyltrimethoxysilane (VTMS), and 2-(dimethylamino)ethyl methacrylate (DMAEMA), described as PDMS-net-P(VTMS-co-DMAEMA). The chemical groups, thermal stability and morphology of this hybrid adsorbent were characterized using techniques of attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR), differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), and scanning electron microscopy (SEM). In adsorption studies, saturation of the active sites of the material was observed at pH 5, after 3 days, with each gram of material capable of adsorbing 0.48 mmol of copper(II). The fractionary-order and Sips models provided the best fits to the experimental data in kinetic and equilibrium studies of the adsorption process, respectively. Moreover, an acceptable reusability was found for this cross-linked organic-inorganic hybrid adsorbent after usage-regeneration cycles without significantly losing its original activity.