Herein, we report a new metal–organic framework (MOF)-based composite beads adsorbent made via incorporating UiO-66 MOF, carboxylated graphene oxide (GOCOOH) into sodium alginate for efficient removal of methylene blue dye, and Cu 2+ ions. The successful fabrication of the synthesized UiO-66/GOCOOH@SA composite beads was confirmed by means of X-ray diffraction, Fourier transform infrared, scanning electron microscopy, zeta potential, X-ray photoelectron spectroscopy analysis, and thermogravimetric analysis and BET measurement. The incorporation of both UiO-66 and GOCOOH into SA beads greatly increased their adsorption efficiency for the removal of both MB and Cu 2+ with maximum adsorption capacities of 490.72 and 343.49 mg/g, respectively. The removal process of both MB and Cu 2+ follows the pseudo-second-order model and Freundlich isotherm model. A plausible adsorption mechanism was discussed in detail. Regeneration tests clarified that the removal efficiencies toward both MB and Cu 2+ remained higher than 87% after five cycles. These results reveal the potentiality of UiO-66/GOCOOH@SA beads as an excellent adsorbent.