Rapid aging of infrastructure systems is currently pervasive in the US and the anticipated cost until 2020 for rehabilitation of aging lifeline will reach 3.6 trillion US dollars (ASCE 2013). Reliable condition or serviceability assessment is critically important in decision-making for economic and timely maintenance of the infrastructure systems. Advanced sensors and nondestructive test (NDT) methods are the key technologies for structural health monitoring (SHM) applications that can provide information on the current state of structures. There are many traditional sensors and NDT methods, for examples, strain gauges, ultrasound, radiography and other X-ray, etc. to detect any defect on the infrastructure. Considering that civil infrastructure is typically large-scale and exhibits complex behavior, estimation of structural conditions by the local sensing and NDT methods is a challenging task. Non-contact and distributed (or full-field) sensing and NDT method are desirable that can provide rich information on the civil infrastructure’s state. Materials with the ability of emitting light, especially in the visible range, are named as luminescent materials. Mechanoluminescence (ML) phenomenon is the light emission from luminescent materials as a response of an induced mechanical stress. ML materials offer new opportunities for SHM that can directly visualize the stress and crack distributions on the surface of structures through ML light emission. Although material research for ML phenomena have been made substantially, applications of the ML sensors to full-field stress and crack visualization are still at infant stage and have yet to be full-fledged. Moreover, practical applications of the ML sensors for SHM of civil infrastructure have difficulties since numerous challenging problems (eg environmental effect) arise in actual applications. In order to realize a practical SHM system employing ML sensors, more research needs to be conducted, for examples, fundamental understandings of physics of ML phenomenon, method for quantitative stress measurements, calibration method for ML sensors, improvement of sensitivity, optimal manufacturing and design of ML sensors, environmental effects of ML phenomenon (eg temperature), image processing and analysis, etc. In this research, fundamental ML phenomena of two most promising ML sensing materials were experimentally studied and a methodology for full-field quantitative strain measurements, for the first time, was proposed along with a standardized calibration method. Characteristics and behavior of ML composites and thin films coated on the structure have been studied under various material tests including compression, tension, pure shear, bending, etc. In addition, ML emission sensitivity to the manufacturing parameters and experimental conditions was addressed in order to find optimal design the ML sensor. A phenomenological stress-optics transduction model for predicting the ML light intensity from a thin-film ML coating sensor subjected to in-plane stresses was proposed. A new full-field quantitative strain measuring methodology by ML thin film sensor was developed, for the first time, in order to visualize and measure the strain field. The results from the ML sensor were compared and verified by finite element simulation results. For NDT applications of ML sensors, experimental tests were conducted to visualize the cracks on structural surfaces and detect damages on structural components. In summary, this research proposes and realizes a new distributed stress sensor and NDT method using ML sensing materials. The proposed method is experimentally validated to be effective for stress measurement …