Theoretical and computational models of neural systems have been traditionally focused on small neural circuits, given the lack of reliable data on large-scale brain structure. The situation has started to change in recent years, with novel recording technologies and coordinated efforts to describe the brain at a larger scale. In this talk, I will review my recent work on developing anatomically constrained computational models of large-scale cortical networks of monkeys, and how this approach can help to answer important questions in large-scale neuroscience. I will focus on three main aspects: (i) the emergence of functional interactions in different frequency regimes, (ii) the role of balance for efficient large-scale communication, and (iii) new paradigms of brain function, such as working memory, in large-scale networks.