 Shapeshifting might sound like the stuff of myth, but to many material scientists it's a very real part of their job. Researchers around the globe are learning how to build the most dynamic and adaptive materials ever conceived, materials that can instantly become more aerodynamic, provide camouflage, or even help people walk again. And the best part, the materials practically build themselves. Using an assortment of chemical schemes, researchers are coding the macroscopic properties of materials directly into microscopic, self-assembling building blocks like these. And with unprecedented processing power at their fingertips, they're using computer simulation to dream up and test new designs. Self-assembly is a universal principle. It is the thermodynamic driving force behind everything from the formation of galaxies to the interlocking of proteins in our bodies. In short, it's nature's way of getting things done. Scientists today are leveraging that same force to piece together the molecular ingredients of functional materials in the lab. Some of the most versatile building blocks look like this. These are polymer-tethered nanoparticles. Like tiny bricks, nanoparticles can be interlocked with a polymer mortar to form superstructures of various shapes, thin sheets, long tubes, and more exotic geometries like this one called a gyroid. And because the nanoparticles and binding polymers themselves possess unique physical and chemical properties, an entire gallery of dynamic materials can be accessed with a few simple building blocks. Take this lattice of gold nanoparticles, for instance. They're bound together by a familiar functional polymer, DNA. By adjusting the length of the DNA strands, scientists can tune the distance between the gold particles. These changes may be incredibly small, but they can drastically alter the optical and electronic properties of the material on the macroscopic scale. The same goes for the rods and coils that form the subunits of this flat polymer sheet. Heating the material causes each coil to contract. The collective motion of billions of these coils is observed as the scrolling of the polymer sheet into a tube. Bringing the tube down to colder temperatures reverses the transformation. Given that a few simple building blocks can give rise to an enormous design space, how can researchers predict the behavior of their macro material? Or perhaps more importantly, how can they tailor their building blocks to create a material for a given application? Over the past decade, researchers have tackled this and other problems by simulating the design process. With the enormous computational capacity of today's processors, scientists can arrange tethered nanoparticles into virtual architectures and predict which designs work best. Working hand-in-hand, therefore, theorists and experimentalists can create tailor-made materials faster than ever. Tethered nanoparticles hold great promise as the structural elements of tomorrow's generation of materials. Stable, programmable, and scalable, they could help researchers craft the right material for practically any job. And with the ability to predict their behavior before taking to the lab, researchers are well equipped to take on the challenge.