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Organic–inorganic hybrid perovskites have been intensively researched in the past decade for their optoelectronic properties. The emergence of Ruddlesden–Popper perovskites, which have mixed dimensionality, has heralded new opportunities for tailor-made semiconductors that combine enhanced stability with useful properties between those of 2D and 3D systems. Inspired by advances in 2D materials research, there is growing interest in molecularly thin versions of these hybrid perovskites, owing to their ease of incorporation into electronic devices. There is, thus, a need to understand thickness-dependent electrical, excitonic and phononic properties that go beyond quantum-confinement effects. Recent studies have shown that, apart from tuning the dimensionality of the system, fine-tuning its thickness also helps to optimize performance in different applications, ranging from third-harmonic generation to …