The adsorption of tetracycline (TC), cadmium [Cd(II)] and arsenate [As(V)] onto magnetic graphene oxide (MGO), magnetic chemically-reduced graphene (MCRG) and magnetic annealing-reduced graphene (MARG) was investigated to understand the adsorption properties and molecular mechanisms. The adsorption of three contaminants was pH-dependent and the adsorption capability followed the order of MGO > MCRG > MARG, and hence MGO was selected to systematically study the adsorption behaviors in three different types of binary systems. The maximum adsorption capacities of MGO were 252 mg/g for TC, 234 mg/g for Cd(II) and 14 mg/g for As(V). The superiority of MGO was mainly attributed to its high dispersibility, thin nanosheets and various O-containing functional groups. In addition to H-bonding and pi-pi interactions, the strong adsorption of TC onto MGO was mainly due to the n-pi electron-donor-acceptor (EDA) effect, with the maximum adsorption around pKa of TC. The mutual effects of TC and Cd(II) in the simultaneously added system were negligible. Adsorption of As(V) was significantly suppressed in the presence of TC, whilst As(V) hardly affected TC adsorption. The adsorptions of Cd(II) and As(V) in the co-adsorption system were increased by 65% and 30%, respectively. This synergistic effect resulted from the electrostatic attraction and the formation of type A ternary surface complexation. These new insights were valuable for elucidating the interaction mechanisms and designing novel adsorbents for traditional and emerging pollutions in practical application.