Understanding the physiological correlates of cognitive overload has implications for gauging the limits of human cognition, developing novel methods to define cognitive overload, and mitigating the negative outcomes associated with overload. Most previous psychophysiological studies manipulated verbal working memory load in a narrow range (an average load of 5 items). It is unclear, however, how the nervous system responds to a working memory load exceeding typical capacity limits. The objective of the current study was to characterize the central and autonomic nervous system changes associated with memory overload, by means of combined recording of electroencephalogram (EEG) and pupillometry. Eighty-six participants were presented with a digit span task involving the serial auditory presentation of items. Each trial consisted of sequences of either 5, 9, or 13 digits, each separated by 2 s. Both theta activity and pupil size, after the initial rise, expressed a pattern of a short plateau and a decrease with reaching the state of memory overload, indicating that pupil size and theta possibly have similar neural mechanisms. Based on the described above triphasic pattern of pupil size temporal dynamics, we concluded that cognitive overload causes physiological systems to reset, and release effort. Although memory capacity limits were exceeded and effort was released (as indicated by pupil dilation), alpha continued to decrease with increasing memory load. These results suggest that associating alpha with the focus of attention and distractor suppression is not warranted.