Rapidly increasing environmental deterioration through heavy metal (HM) ions’ accumulation calls for highly efficient, facile, and sustainable remediation techniques. Adsorption mechanism for HM ions removal, although existed for many decades, yet the conventional carbon materials as adsorbents are unable to provide satisfactory output. Amongst different carbon-based emerging materials, graphene-based nanomaterials (NMS) are playing a pivotal role in diverse fields, including environmental remediation. Graphene NMS possess immense surface area, superior electronic conductivity, high mechanical strength, and numerous surface functional groups, conferring them superior attributes as an adsorbent material. The current chapter explores the different properties and forms of graphene suitable for HM ions adsorption. Further, the process of HM ions adsorption about different metals such as arsenic (As), lead (Pb), chromium (Cr), cadmium (Cd), copper (Cu), and mercury (Hg) has been elaborated along with the involved adsorption kinetics and adsorptive isotherm mechanism. At the end, different forces involved in the adsorptive activity of graphene-NMS have been discussed.