Various graphene-based nanoadsorbents, including graphenes, graphene oxides, reduced graphene oxides, and their nanocomposites, have been widely studied as potential adsorbents due to their unique physicochemical properties, such as structural variability, chemical strength, low density, and the possibility of large scale fabrication. Adsorption mechanisms are governed largely by the physicochemical properties of contaminants, the characteristics of nanoadsorbents, and background water quality conditions. This review summarizes recent comprehensive studies on the removal of various inorganic (mainly heavy metals) and organic contaminants by graphene-based nanoadsorbents, and also discusses valuable information for applications of these nanoadsorbents in water and wastewater treatment. In particular, the aqueous removal of various contaminants was reviewed to (i) summarize the general adsorption capacities of various graphene-based nanoadsorbents for the removal of different inorganic and organic contaminants, (ii) evaluate the effects of key water quality parameters such as pH, temperature, background major ions/ionic strength, and natural organic matter on adsorption, (iii) provide a comprehensive discussion of the mechanisms that influence adsorption on these nanoadsorbents, and (iv) discuss the potential regeneration and reusability of nanoadsorbents. In addition, current challenges and future research needs for the removal of contaminants by graphene-based nanoadsorbents in water treatment processes are discussed briefly.