Organic-inorganic hybrids incorporating cellulose/silica carrier particles functionalized with tetraethylene-pentamine (SiO2@Cel-TEPA) were synthesized for the sensing and sequestering of Cu(II) ions from contaminated waters with high-performance naked eye sensing and efficient removal. The modification of the SiO2@Cel nanocomposite was carried out through simultaneous treatment with POCl3 followed by decoration with tetraethylenepentamine to obtain SiO2@Cel-TEPA optical mesocaptor. The existence and uniform distribution of silica onto cellulose fibers and the success of the optical mesocaptor synthesis were investigated by means of elemental analysis, Fourier transfrom infrared and Raman spectroscopies, N-2 adsorption-desorption, scanning electron microscopy, energy-dispersive spectrometry, high-resolution transmission electron microscopy, and differential thermal analysis/thermogravimetic analysis measurements. On the basis of our results, the fabricated SiO2@Cel-TEPA material displays a significant Cu(II) ion-sensing capability even at trace concentrations, maintaining functionality for reuse and recycle using simple decomplexation without significant deterioration in its original performance.