Monolayer-protected gold nanoparticles have many appealing physical and chemical properties such as quantum size effects, surface plasmon resonance, and catalytic activity. These hybrid organic-inorganic nanomaterials have promising potential applications as building blocks for nanotechnology, as catalysts, and as sensors. Recently, the chirality of these materials has attracted attention, and application to chiral technologies is an interesting perspective. This minireview deals with the preparation of chiral gold nanoparticles and their chiroptical properties. On the basis of the latter, together with predictions from quantum chemical calculations, we discuss different models that were put forward in the past to rationalize the observed optical activity in metal-based electronic transitions. We furthermore critically discuss these models in view of recent results on the structure determination of some gold clusters as well as ligand-exchange experiments examined by circular dichroism spectroscopy. It is also demonstrated that vibrational circular dichroism can be used to determine the structure of a chiral adsorbate and the way it interacts with the metal. Finally, possible applications of these new chiral materials are discussed.