Hybrid organic-inorganic perovskite materials have become one of the leading semiconductors for renewable solar-to-electric energy conversion in photovoltaics. However, they are unstable under operating conditions, which stimulates global research efforts to overcome this challenge towards practical applications. Supramolecular strategies have provided an invaluable tool for controlling hybrid perovskite materials by purposefully tailoring noncovalentninteractions with organic components, such as through halogen bonding, π- interactions, and host-guest complexation, which has been assessed at the atomic level by solid-state NMR spectroscopy. These strategies were also applied to the development of low-dimensional perovskite architectures that further enhance stabilities as well as photovoltaic performances.As a result, perovskite solar cells have reached superior operational stabilities without compromising their performances,providing a versatile strategy for advancing hybrid photovoltaics.

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