At any time, we are processing thousands of stimuli, but only few of them will be remembered hours or days later. Is there any way to predict which ones? Here, we tested whether the pupil response to ongoing stimuli, an indicator of physiological arousal known to be relevant for memory formation, is a reliable predictor of long-term memory for these stimuli, over at least 1 day. Pupil dilation was tracked while participants performed visual and auditory encoding tasks. Memory was tested immediately after encoding and 24 hr later. Irrespective of the encoding modality, trial-by-trial variations in pupil dilation predicted reliably which stimuli were recalled in the immediate and 24 hr-delayed tests, in particular for emotionally arousing stimuli. These results show that our eyes may provide a window into the formation of long-term memories. Furthermore, our findings underline the important role of central arousal systems in the rapid formation of memories in the brain, possibly by gating synaptic plasticity mechanisms in the neocortex.