Herein, we report the first example of supramolecular carbon nanotube (CNT)-based ion catchers as simple and effective tools for removing divalent metal ions from organic solvents. In particular, covalently functionalized multi-walled carbon nanotubes (MWCNTs) appended with pyridyl groups self-aggregate in solution into bundles in the presence of divalent metal ions (e.g., Cd2+, Cu2+, Ni2+, Pb2+, Zn2+). Such self-aggregation behavior leads to insoluble materials that, upon treatment with weak acids, can be regenerated and reused for further complexation. All materials and complexation/decomplexation steps were thoroughly characterized by using X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), and different microscopy-based techniques, namely, transmission electron, scanning electron, and atomic force microscopy (TEM, SEM, and AFM). The supramolecular system engineered in this work is the first example of an easy and fully sustainable material with great potential applications for depolluting liquid waste from metal contamination.