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Reliability is essential for large-scale applications of high-power light-emitting diode (LED) devices, modules, and systems for general illumination. In this paper, the reliability of a novel application-specific LED package (ASLP) is investigated by thermal shock testing, failure analysis, and fluid-solid coupling thermo-mechanical simulation. The reliability of the ASLP modules was validated with a dual-bath liquid thermal shock testing from 233 to 398 K. The non-destructive failure analysis was conducted to the catastrophic failure ASLP samples by fluorescent penetrant inspection. The delaminations at the interfaces within the ASLP module were detected. The failure mechanisms were identified by digital optical microscopy and field emission scanning electron microscope inspection after the decapsulation. The experimental results show that fracture failure occurs at the wedge joint of the bonding wire, which leads to the catastrophic failure of the ASLP module. The stress and strain behaviors of the ASLP module, especially the bonding wire under thermal shock loading, were analyzed through thermo-mechanical modeling with the nonlinear time- and temperature-dependent material properties. Significant thermal gradient within the ASLP module during the thermal shock testing was taken into consideration by the fluid-solid coupling transient thermal transfer analysis. The effects of the delaminations detected by the fluorescent penetrant inspection on the reliability of the bonding wire were also examined. It is found the delaminations existing at the interfaces within the ASLP module induce significant plastic strain to the wedge joint and results in fracture failure. The results from the numerical simulation can make a good prediction of the failure mechanism of the ASLP modules under thermal shock loading.