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Brillouin scattering-based distributed fiber optic sensing (Brillouin-DFOS) technology is widely used in health monitoring of large-scale structures with the aim to provide early warning of structural degradation and timely maintenance and renewal. Material cracking is one of the key mechanisms that contribute to structural failure. However, the conventional strain measurement using the Brillouin-DFOS system has a decimeter-order spatial resolution, and therefore it is difficult to measure the highly localized strain generated by a sub-millimeter crack. In this study, a new crack analysis method based on Brillouin scattering spectrum (BSS) data is proposed to overcome this spatial resolution-induced measurement limitation. By taking the derivative of the BSS data and tracking their local minimums, the method can extract the maximum strain within the spatial resolution around the measurement points. By comparing the variation of the maximum strain within the spatial resolution around different measurement points along the fiber, cracks can be located. The performance of the method is demonstrated and verified by locating and quantifying a small gap created between two wood boards when one of the wood boards is pushed away from the other. The test result verifies the accuracy of the crack strain quantification of the method and proves its capability to measure a sub-millimeter crack. The method is also applied to a thin bonded concrete overlay of asphalt pavement field experiment, in which the growth of a transverse joint penetrating through the concrete–asphalt interface was monitored. The method successfully locates the position, traces the strain variation, and estimates the width of a crack less than [Formula: see text] wide using a Brillouin-DFOS system with [Formula: see text] spatial resolution.