Organic–inorganic layered perovskites were initially
envisioned
as materials for solar cells in view of their greater ambient stability
compared to their 3D relatives. However, their major limitation was
the insulating character of the bulky organic cations, especially
in single-layer structures. This limitation was turned into an opportunity
to explore organic molecules with different configurations, a journey
that, to date, has delivered new materials for lighting, photocatalysis,
chiro-optoelectronics, and ferroelectricity. In this Perspective,
we aim to provide an outlook on the future challenges of using metal-halide
Ruddlesden–Popper layered perovskites as scaffolds, including
functional organic building blocks, for the creation of new hybrid
materials. We envision that this research field can be empowered by
establishing strong bridges with the organic chemistry and the machine-learning
communities, which will help researchers to efficiently design new
organic cations for exciting functionalities in this class of materials.