Materials nanoarchitectonics has led to important innovations in the design and construction of systems in nanoelectronics, nanomachinery, and energy conversion. Recent publications point to the fact that the same approach may be applied successfully to other fields. In this Perspective, we define the key features of materials nanoarchitectonics and examine how they can be used to address current challenges in nanomedicine, placing emphasis on colloidal agents for therapeutic and diagnostic applications.