<p>Cancer, a leading cause of global mortality, demands the development of targeted therapies due to rising treatment resistance and limited efficacy of current drugs. N-heterocyclic carbenes (NHCs) represent a unique class of ligands, primarily due to their strong σ-donor and weak π-acceptor properties, making them highly valuable in organometallic and medicinal chemistry. The metal-NHC complexes are prepared by reacting the respective azolium salts with the appropriate metal sources. In recent years, metal complexes have gained considerable attention for their promising cytotoxic activity, particularly NHC-based metal complexes that demonstrate superior anticancer efficacy compared to conventional chemotherapeutic agents. This review provides a comprehensive overview of advances made over the past five years in organoselenium and silver-NHC complexes derived from (benz)imidazole, highlighting their significant potential in anticancer applications. The antitumor activities, proposed mechanisms of action, and structure–activity relationships of NHC-based metallodrugs are systematically reviewed. We hope this review inspires researchers to design novel metal-based NHC compounds for cancer treatment.</p> Graphical Abstract <p></p>