Rapid industrialization has resulted in serious heavy metal pollution. The removal of heavy metal ions from solutions is very important for environmental safety and human health. Poly (amidoamine) (PAMAM) dendrimers are artificial macromolecular materials with unique physical and chemical properties. Abundant amide bonds and amino functional groups provide them with a high affinity for heavy metal ions. Herein, PAMAM-functionalized adsorbents are reviewed in terms of different nanomaterial substrates. Approaches in which PAMAM is grafted onto the surfaces of substrates are described in detail. The adsorption isotherms and kinetics of these adsorbents are also discussed. The effects of PAMAM generation, pH, adsorbent dosage, adsorption time, thermodynamics, and ionic strength on adsorption performance are summarized. Adsorption mechanisms and the further functionalization of PAMAM-grafted adsorbents are reviewed. In addition to the positive results, existing problems are also put forward in order to provide a reference for the optimization of PAMAM-grafted adsorbents of heavy metal ions.