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Recently, supershear Rayleigh waves (SRWs) have been proposed to characterize the biomechanical properties of soft tissues. The SRWs propagate along the surface of the medium, unlike surface Rayleigh waves, SRWs propagate faster than bulk shear waves. However, their behavior and application in biological tissues is still elusive. In brain tissue elastography, shear waves combined with magnetic resonance elastography or ultrasound elastography are generally used to quantify the shear modulus, but high spatial resolution elasticity assessment in 10 μm scale is still improving. Here, we develop an air-coupled ultrasonic transducer for noncontact excitation of SRWs and Rayleigh waves in brain tissue, use optical coherent elastography (OCE) to detect, and reconstruct the SRW propagation process; in combing with a derived theoretical model of SRWs on a free boundary surface, we quantify the shear modulus of brain tissue with high spatial resolution. We first complete validation experiments using a homogeneous isotropic agar phantom, and the experimental results clearly show the SRW is 1.9649 times faster than the bulk shear waves. Furthermore, the propagation velocity of SRWs in both the frontal and parietal lobe regions of the brain is all 1.87 times faster than the bulk shear wave velocity. Finally, we evaluated the anisotropy in different brain regions, and the medulla oblongata region had the highest anisotropy index. Our study shows that the OCE system using the SRW model is a new potential approach for high-resolution assessment of the biomechanical properties of brain tissue.