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Strain engineering, as a non‐chemical tuning knob, can enhance the performance of semiconductor devices. Here, an efficient manipulation of light emission is revealed in thin‐layered 2D perovskite strongly correlated to layer numbers of [PbI6]4− octahedron (n) and [C6H5(CH2)2NH3]2(CH3NH3)n‐1PbnI3n+1 (N) by applying uniaxial strains (ɛ) via bending the flexible substrate. As increases from 1 to 3, an efficient light emission redshift (ɛ from −0.97% to 0.97%) is observed from bandgap shrinkage, and the shrinkage rate increases from 1.97 to 10.38 meV/%, which is attributed to the predominant uniaxial intralayer deformation due to the anisotropy of the [PbI6]4− octahedron lattice strain. Conversely, as increases from 7 to 48 for n = 3, the deformation related to bandgap shrinkage rate is more prominent in small‐N flakes ( ≈ 7, 15.2 meV/%) but is easily offset in large‐N flakes ( ≈ 48, 7.7 meV/%). This anisotropic lattice deformation, meanwhile, inevitably modulates the carrier recombination dynamics of [C6H5(CH2)2NH3]2(CH3NH3)n‐1PbnI3n+1, which is essential for the development of highly efficient photoelectronic devices. [ABSTRACT FROM AUTHOR]

The island‐bridge structural design is a common strategy for imparting stretchability to flexible electronic devices. In this structure, the low modulus regions bear most of the deformation, while the rigid islands, which house the electronic components, undergo minimal deformation. However, due to the modulus differences that can be several times or even several orders of magnitude larger, severe strain concentration occur at the edges of the rigid islands in high modulus regions. This strain concentration caused by rigid constraints not only reduces the stretchability of the soft substrate but also degrades the mechanical performance of the interconnected structures, thereby significantly affecting the overall stability of the device. Starting from finite element simulations, this paper introduces modulus gradient regions and optimizes geometric parameters, significantly alleviating the strain concentration at the edges of the rigid islands. Serpentine‐shaped circuits are then transferred to a substrate with strain isolation, which demonstrates better stretchability stability under 20% elongation compared to traditional strain isolation strategies. In addition, the stretchable light emitting diode (LED) system with gradient modulus has better stretchability compared to the system with conventional strategy. This suggests that this strategy has great potential in maintaining the stability of stretchable systems. [ABSTRACT FROM AUTHOR]