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Highly efficient adsorbents, which can effectively remove both metal ions and dyes from wastewater with robust stability, are strongly required for the remediation of current polluted aqueous system, but still a challenge to be realized. Herein, a new adsorbent has been designed to solve this problem by anchoring diethylene triamine pentaacetic acid (DTPA) grafted polyethyleneimine (PEI) onto carboxylated GO (GOC-g-PD). Given the amino and carboxyl active groups from PEI and GOC/DTPA, our GOC-g-PD displays good adsorption capacity against not only inorganic metal ions (Cu2+ and Pb2+) but also organic dye (methylene blue: MB). The maximum adsorption capacity of GOC-g-PD for Cu2+, Pb2+ and MB reached 309.60 mg·g−1, 316.17 mg·g−1 and 262.10 mg·g−1, respectively. Furthermore, our GOC-g-PD also exhibits good cycling stability and chemical stability against wide pH values. These outstanding properties revealed our GOC-g-PD held great potential in purifying the sewage discharged from industries. [ABSTRACT FROM AUTHOR]