In the past decades, atomically controlled multicomponent nanomaterials have served as platforms to advance the understanding of scientific phenomena along with providing practical solutions for various applications. Colloidal chemistry and atomic layer deposition techniques are two of the most powerful techniques to tailor make materials with tunable composition and morphology. In this Review, we focus on how the combination of these two highly versatile chemistries enables an atomic-scale of multicomponent nanomaterials in a wide compositional range. We discuss very recent studies from us and others, which encourage the scientific community to explore the tunability offered by such combination even further.