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Cognitive function relies on the dynamic cooperation of specialized regions of the brain; however, the elements of the system responsible for coordinating this interaction remain poorly understood. In this Opinion article I argue that this capacity is mediated in part by competitive and cooperative dynamic interactions between two prominent metabotropic neuromodulatory systems – the cholinergic basal forebrain and the noradrenergic locus coeruleus (LC). I assert that activity in these projection nuclei regulates the amount of segregation and integration within the whole brain network by modulating the activity of a diverse set of specialized regions of the brain on a timescale relevant for cognition and attention.