The ability to allocate and maintain visual attention enables us to adaptively regulate perception and action, guiding strategic behaviour within complex, dynamic environments. This capacity to regulate attention develops rapidly over the early years of life, and underpins all subsequent cognitive development and learning. From screen-based experiments we know something about how attention control is instantiated in the developing brain, but we currently understand little about the development of the capacity for attention control within complex, dynamic, real-world settings. To address this, we recorded brain activity, autonomic arousal and spontaneous attention patterns in N=58 5- and 10-month-old infants during free play. We used time series analyses to examine whether changes in autonomic arousal and brain activity anticipate attention changes or follow on from them. Early in infancy, slow-varying fluctuations in autonomic arousal forward-predicted attentional behaviours, but cortical activity did not. By later infancy, fluctuations in fronto-central theta power associated with changes in infants’ attentiveness and predicted the length of infants’ attention durations. But crucially, changes in cortical power followed, rather than preceded, infants’ attention shifts, suggesting that processes after an attention shift determine how long that episode will last. We also found that changes in fronto-central theta power modulated changes in arousal at 10 but not 5 months. Collectively, our results suggest that the modulation of real-world attention involves both arousal-based and cortical processes but point to an important developmental transition. As development progresses, attention control systems become dynamically integrated and cortical processes gain greater control over modulating both arousal and attention in naturalistic real-world settings.