The present study is the first to examine individual differences in long-term memory, arousal dysregulation, and intensity of attention within the same experiment. Participants (N = 106) completed 28 lists of an immediate free recall task while their pupil diameter was recorded via an eye-tracker during the encoding period. Two main pupillary measures were extracted: intraindividual variability in pre-list pupil diameter and evoked pupillary responses during item encoding. Variability in pre-list pupil diameter served as a measure of arousal dysregulation, and evoked pupillary responses served as a measure of intensity of attention. Based on prior work, we hypothesized that there would be a positive association between intensity of attention and recall ability, and that there would be a negative association between arousal dysregulation and recall ability. Collectively these two measures accounted for 19% of interindividual variance in recall, with 5% attributable uniquely to intensity of attention and 12% attributable uniquely to arousal regulation. The findings demonstrate that there are sources of individual differences in long-term memory that can be revealed via pupillometry, notably the amount of effort deployed during item encoding and the degree to which people exhibit dysregulated arousal. Both findings are consistent with recent theorizing regarding the role of the locus coeruleus-norepinephrine (LC-NE) system’s role in goal-directed cognition. Specifically, the LC governs both moment-to-moment arousal and NE release to cortical regions subserving cognitive processing. Among people for whom this system operates most optimally, long-term memory retention is superior.