This work focuses on the sequestration of Cu(II) from aqueous environment owing to the risks posed to human health. A magnetic hybrid aerogel (mGO‐TETA‐MWCNT) was synthesized by one‐pot self‐assembly of magnetic graphene oxide (mGO) and multiwalled carbon‐nanotubes (MWCNT) post functionalization with triethylenetetramine (TETA) through hydrothermal reduction. The prepared adsorbent was characterized and employed for efficient removal of Cu(II). The aerogel, mGO‐TETA‐MWCNT presented maximum adsorption capacity (Qmax) of 232.22 mg g−1 at Box‐Behnken design optimized conditions: pH 5.6, time 36.7 min, and concentration 999.7 mg L−1. The Brouers‐Sotolongo (BS) isotherm and Fractal‐like pseudo‐second‐order (FLPSO) kinetic model fitted best representing heterogeneity of the hybrid adsorbent. The presence of interferent metal ions(Ni(II), Pb(II), Cd(II), Zn(II)) showed negligible effect on the selective sorption of Cu(II). The prepared adsorbent could be regenerated upto five cycles (>95 % removal) when eluted using 0.5 m HCl. The aerogel was successfully utilized to remove Cu(II) from wastewater, river‐water, and groundwater.