Smart luminescent materials have recently received significant attention for applications in sensing, optical displays, biological imaging, and therapy. Construction of host-guest self-assembled structures has been an effective way to achieve such luminescent systems. Here, recent advances in layered double hydroxides (LDHs)-based smart luminescence and the tuning of their excited states are reviewed. We introduce the relationship between the structures and luminescent performance of the LDHs’ host-guest materials and their sensor properties. Then, we focus on the tuning of singlet and/or triplet excited states of the LDHs-based luminescent materials. Finally, we briefly review new host-guest fluorescent and long-lived phosphorescent materials with stimuli-responsive behavior.
