Nicola Marzari, head of the Theory and Simulation of Materials laboratory at EFPL and director of NCCR MARVEL, has just published a review of electronic-structure methods as part of a special edition Insight on Computational Materials Design, published by Nature Materials. The article, written with Andrea Ferretti of CNR–Instituto Nanoscienze and Chris Wolverton of Northwestern University, provides an overview of these methods, discusses their application to the prediction of materials properties, and examines different strategies used to target the broader goals of materials design and discovery. Looking ahead, the authors consider emerging challenges in the predictive accuracy of the calculations, and in addressing the real-life complexity of materials and devices. They also stress the importance of the computational infrastructures that support such research, and how the planning for funding these and the supporting career models is only just beginning to emerge.