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Before such advances are realized, a fundamental understanding of the technical properties of HOIPs is required. Right here, we combine ab initio thickness functional theory (DFT) modeling with a diverse group of experiments to analyze the flexible properties of (quasi)2D HOIPs. Especially, we focus on (quasi)2D solitary crystals of phenethylammonium methylammonium lead iodide, (PEA)2PbI4(MAPbI3)n-1, and their particular 3D counterpart, MAPbI3. We utilized nanoindentation (both Hertzian an