We present a general strategy for a facile synthesis of complex multifunctional nanoscale materials via colloidal atomic layer deposition (c-ALD). The c-ALD technique is based on self-limiting half-reactions of ionic precursors on the surface of a nanocrystal (NC) occurring at room temperature. Using this technique, uniform layers of CdS and ZnS semiconductor shells were epitaxially grown on CdSe semiconductor cores with different shell combinations, leading to the precise control of the optical properties of these heterostructures. All core-shell multicomponent nanoparticles preserve narrow size distributions, phase crystallinity, and shape homogeneity of the initial NCs. Furthermore, we attempted to extend the toolbox of the c-ALD to combine materials with intrinsically different properties, such as Au/CdS core/shell structures with substantial lattice mismatch. The results presented in this work demonstrate great opportunities for creating functional materials with programmable properties for electronics and optoelectronics.