Lossy-mode-resonance (LMR) is a surface plasmon resonance (SPR)-analogue optical phenomenon, which is sensitive to the surrounding environment variations and can be considered as an important detection signal in biochemical sensors. Compared with the SPR sensor which can only operate under transverse magnetic (TM)-polarized light, the LMR sensor shows a more excellent application prospect and can operate in both TM- and transverse electric (TE)-polarized light. In this work, a CH3NH3PbBr3-based LMR configuration is proposed to apply in optical sensors. When the incident light is in TM mode, the preferred way to improve the performance of the LMR sensor is optimizing the thickness of the matching layer, and the highest sensitivity of 11382 refractive index unit (RIU−1) is achieved, which is more than 200 times larger than that of the conventional Au-based SPR sensor; when the incident light is in TE mode, it is more advantageous to improve the properties of LMR sensor by optimizing the thickness of CH3NH3PbBr3 layer, and a high sensitivity of 21697 RIU−1 is obtained. With such high sensitivity, we believe that the CH3NH3PbBr3-based LMR sensor will find potential applications in biology, medicine, chemistry and other fields.