Perovskite single crystals are actively studied as X-ray detection materials with enhanced sensitivity. Moreover, the feasibility of using perovskites for self-powered devices such as photodetectors, UV detectors, and X-ray detectors can significantly expand their application range. In this work, the charge carrier transport and photocurrent properties of MAPbBr₃ single crystals (MSCs) are improved by the mechanochemical surface treatment using glycerin combined with an additional electrode design that forms an ohmic contact. The sensitivity of MSC-based detectors and pulse shape generated by X-rays are enhanced at various bias voltages. The synthesized MSC detectors generate direction-dependent photocurrents, which indicate the presence of a polarization-induced internal electric field. In addition, photocurrent signals are produced by X-rays with energies greater than 1 MeV under a zero-bias voltage. This work demonstrates a high application potential of perovskites as self-powered detectors for X-rays with energies exceeding 1 MeV.