Over the past decade, scientific interest in the properties of large-scale spontaneous neural dynamics has intensified. Concurrently, novel technologies have been developed for characterizing the connective anatomy of intra-regional circuits and inter-regional fiber pathways. It will soon be possible to build computational models that incorporate these newly detailed structural network measurements to make predictions of neural dynamics at multiple scales. Here, we review the practicality and the value of these efforts, while at the same time considering in which cases and to what extent structure does determine neural function. Studies of the healthy brain, of neural development, and of pathology all yield examples of direct correspondences between structural linkage and dynamical correlation. Theoretical arguments further support the notion that brain network topology and spatial embedding should strongly influence network dynamics. Although future models will need to be tested more quantitatively and against a wider range of empirical neurodynamic features, our present large-scale models can already predict the macroscopic pattern of dynamic correlation across the brain. We conclude that as neuroscience grapples with datasets of increasing completeness and complexity, and attempts to relate the structural and functional architectures discovered at different neural scales, the value of computational modeling will continue to grow.