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Nanostructural hybrid organic-inorganic metal halide perovskites offer a wide range of potential applications including photovoltaics, solar cells, and light emitting diodes. Up to now the surface stabilizing ligands were used solely to obtain the optimal properties of nanoparticles in terms of dimensionality and stability, however their possible additional functionality was rarely considered. In the present work, hybrid lead bromide perovskite nanoparticles (PNP) were prepared using a unique approach where a peptide nucleic acid is used as a surface ligand. Methylammonium lead bromide perovskite colloidal nanoparticles stabilized by thymine-based peptide nucleic acid monomer (PNA-M) and relevant trimer (PNA-T) were prepared exhibiting the size below 10 nm. Perovskite structure and crystallinity were verified by X-ray powder diffraction spectroscopy and high resolution transmission electron microscopy. PNP-PNA-M and PNP-PNA-T colloidal dispersions in chloroform and toluene possessed green-blue fluorescence, while Fourier-transform infrared spectroscopy (FT-IR) and quantum chemical calculations showed that the PNA coordinates to the PNP surface through the primary amine group. Additionally, the sensing ability of the PNA ligand for adenine nucleic acid was demonstrated by photoluminescence quenching via charge transfer. Furthermore, PNP thin films were effectively produced by the centrifugal casting. We envision that combining the unique, tailored structure of peptide nucleic acids and the prospective optical features of lead halide perovskite nanoparticles could expand the field of applications of such hybrids exploiting analogous ligand chemistry. Version of record

X‐ray detectors play a pivotal role in development and advancement of humankind, from far‐reaching impact in medicine to furthering the ability to observe distant objects in outer space. While other electronics show the ability to adapt to flexible and lightweight formats, state‐of‐the‐art X‐ray detectors rely on materials requiring bulky and fragile configurations, severely limiting their applications. Lead halide perovskites is one of the most rapidly advancing novel materials with success in the field of semiconductor devices. Here, an ultraflexible, lightweight, and highly conformable passively operated thin film perovskite X‐ray detector with a sensitivity as high as 9.3 ± 0.5 µC Gy−1 cm−2 at 0 V and a remarkably low limit of detection of 0.58 ± 0.05 μGy s−1 is presented. Various electron and hole transporting layers accessing their individual impact on the detector performance are evaluated. Moreover, it is shown that this ultrathin form‐factor allows for fabrication of devices detecting X‐rays equivalently from front and back side., Ultraflexible, lightweight, and highly conformable thin film perovskite X‐ray detectors are presented here. An evaluation of the individual impact on the detector performance of various electron and hole transporting layers is provided. Such devices are passively operated and show a high sensitivity and a remarkably low limit of detection, allowing also for isotropic detection.