As a thermal interface material, diamond/GaInSn composites have wide-ranging application prospects in the thermal management of chips. However, studies on systematic reliability that can guide the practical application of diamond/GaInSn in the high-temperature, high-temperature impact, or high-humidity service environments that are faced by chips remain lacking. In this study, the performance evolution of diamond/GaInSn was studied under high-temperature storage (150 °C), high- and low-temperature cycling (−50 °C to 125 °C), and high temperature and high humidity (85 °C and 85% humidity). The experimental results reveal the failure mechanism of semi-solid composites during high temperature oxidation. It is revealed that core oxidation is the key to the degradation of liquid metal composites’ properties under high-temperature storage and high- and low-temperature cycling conditions. Under the conditions of high temperature and high humidity, the failure of Ga-based liquid metal and its composite materials is significant. Therefore, the material should avoid high-temperature and high-humidity environments.