[EN] In this work, we unravel the photodynamics of Nile Red (NR) interacting with Al-ITQ-HB nanostructure, a new layer-type metal-organic framework (MOF) with potential catalytic and photonic applications. Steady-state spectroscopy reveals the presence of NR monomers and aggregates when interacting with the MOF structure. Time-resolved experiments provide emission lifetimes of the interacting monomers, H-and J-type aggregates. We observed contributions from two monomer populations having different environments. One monomer species emits from the local-excited state and another from a photo-produced charge-separated state resulting from an ultrafast intramolecular charge transfer (ICT). Femtosecond fluorescence experiments reveal that the IC...