The invention discloses a quantum magneto-optical sensor, and relates to the field of quantum-level ultra-micro detection sensors of nuclear magnetic resonance and Raman spectrum, in particular to a quantum magneto-optical sensor in states of nuclear magnetic magnetization, nuclear magnetic resonance, nuclear magnetic relaxation and nuclear magnetic non-magnetization. According to the method, the distribution probability difference of Raman scattering light in orientation and direction caused by electron level transition of specific protons in an object is detected, the optimal magneto-optical included angle of exciting light and the Raman scattering light is searched and adjusted, higher Raman scattering light collection efficiency is obtained, a characteristic magnetic spectrum and a characteristic spectrum are collected at the same time, and according to quantum correlation, the Raman scattering light collection efficiency is improved. More information can be found out from quantum correlation, specifically, a quantum magneto-optical sensor is composed of a main magnetic field generator, an excitation induction coil, a control subsystem, a laser and a Raman probe, the magneto-optical included angle is adjusted in an off-axis mode or a coaxial mode, the Raman spectrum collection efficiency is improved, and the detection accuracy is improved. Meanwhile, association of the characteristic magnetic spectrum and the characteristic spectrum in multiple states is realized, and a calculation basis is provided for further analyzing and detecting the content of molecules.