Heavy metals represent one of the most important kinds of pollutants, causing serious threats to the ecological balance. Thus, their removal from aqueous solution is a major environmental concern worldwide. The process of adsorption—being very simple, economical, and effective—is widely applied for the decontamination of wastewaters from heavy metals. In this process, the adsorbent is the key factor affecting the performance; for this reason, significant efforts have been made to develop highly efficient and selective adsorbents with outstanding properties. This paper presents a detailed overview of the research on different methods of synthesis of nanocomposite materials based on the polymer polyaniline combined with nanomaterials, along with the influence of the synthesis method on their size, morphology, and properties. In addition, the study evaluates the adsorption efficiency of various developed nanocomposites for the adsorption of heavy metals from aqueous solution. From an economical and environmental point of view, the regeneration studies of the nanocomposites are also reported.