Recent advances in neuroanatomy and physiology make it possible to probe whole-brain mechanisms of cognition and behavior. However, as yet, few models in computational neuroscience have tackled the mechanisms underlying highly distributed neural activity during cognitive tasks. In this talk I will describe our anatomy-led approach to developing cortex-wide models of neural dynamics during cognitive tasks and our recent anatomical findings of gradients of neurotransmitter receptors in the cortex. I will highlight our investigations into how inputs from neuromodulatory systems may shift the cortical dynamical landscape, affecting cell-type specific interactions, and how this may confer flexibility on distributed cognitive functions such as conscious perception and working memory.