Attention can be directed not only to sensory stimuli from the external environment but also to internal representations in memory. While attentional selection in working memory (WM) has been widely studied, we know less about how we focus on contents within long-term memory (LTM). In two experiments, we directly compared the consequences of selecting items in LTM and WM, examining influences on subsequent recall and perception. Participants first learned the features of two LTM items during a learning phase. In the subsequent phase, participants viewed two items with features different from the LTM items and encoded these into WM. After a delay, a retrocue informed participants which item they should select from either the LTM or WM items or, was uninformative. On half of the trials, participants were prompted to recall the retrocued item. Critically, on the other trials, participants performed a perceptual discrimination task on a briefly presented and masked sensory array unrelated to the memory contents. The item to discriminate appeared equiprobably at the four locations, thereby overlapping with retrocued LTM or WM locations on 25% of the trials. In both experiments, informative retrocues facilitated recall speed for LTM and WM contents. Retrocuing items in LTM and WM also incidentally improved perceptual discrimination for visual items coinciding with the location of retrocued items, despite retrocues having no sensory predictive value. Although the behavioural benefits showed a similar pattern, eye tracking suggested functionally dissociable mechanisms for orienting attention in LTM and WM. Significant gaze biases followed retrocues indicating items in WM but not in LTM. Overall, our study introduces an experimental approach for comparing the processes and consequences of attentional orienting in LTM and WM. We observe memory and perceptual benefits for attentional orienting in both memory domains but through partially dissociable mechanisms.