Separation-free Al-Mg/graphene oxide (Al-Mg/GO) composites were synthesized by facile one-pot hydrothermal treatment and examined for adsorptive removal of representative contaminants (phosphate, copper (II), and Diclofenac (DCF)) in urban stormwater runoff. The Al-Mg/GO composites exhibited good adsorption capacity for all three contaminants. The adsorption isotherm and kinetics are well described by Freundlich model and pseudo-second-order model, respectively. Further, adsorption of phosphate and DCF favored acidic conditions while an opposite trend was observed for copper (II), which can be ascribed to the change of surface charge of the composites at different pH. The presence of different ions commonly present in environmental matrices (humic acid, bicarbonate, and sulfate) exhibited different effects on the contaminants' removal. Bicarbonate inhibited phosphate and DCF adsorption but promoted copper (II) removal. Copper (II) adsorption was also increased through chemical complexation and electrostatic attraction as a result of humic acid/sulfate adsorption on the adsorbents. The adsorption mechanisms include electrostatic interaction for all three contaminants, Lewis acid-base interactions and surface complexation for phosphate, π-π interactions for DCF, and cation-π interactions for copper (II). More than 75% adsorption capacities were maintained after 4 cycles of adsorption/desorption/regeneration, indicating good reusability. The Al-Mg/GO composites show great potential as a multifunctional adsorptive material for urban stormwater management.