Executive control (EC) generally refers to the regulation of mental activity. It plays a crucial role in complex cognition, and EC skills predict high-level abilities including language processing, memory, and problem solving, as well as practically relevant outcomes such as scholastic achievement. EC develops relatively late in ontogeny, and many sub-groups of developmental populations demonstrate an exaggeratedly poor ability to control cognition even alongside the normal protracted growth of EC skills. Given the value of EC to human performance, researchers have sought means to improve it through targeted training; indeed, accumulating evidence suggests that regulatory processes are malleable through experience and practice. Nonetheless, there is a need to understand both whether specific populations might particularly benefit from training, and what cortical mechanisms engage during performance of the tasks used in the training protocols. This contribution has two parts: in Part I, we review EC development and intervention work in select populations. Although promising, the mixed results in this early field make it difficult to draw strong conclusions. To guide future studies, in Part II, we discuss training studies that have included a neuroimaging component - a relatively new enterprise that also has not yet yielded a consistent pattern of results post-training, preventing broad conclusions. We therefore suggest that recent developments in neuroimaging (e.g., multivariate and connectivity approaches) may be useful to advance our understanding of the neural mechanisms underlying the malleability of EC and brain plasticity. In conjunction with behavioral data, these methods may further inform our understanding of the brain-behavior relationship and the extent to which EC is dynamic and malleable, guiding the development of future, targeted interventions to promote executive functioning in both healthy and atypical populations.