In recent years, we have developed a series of gallium-based liquid metal pastes containing low content solid metal particle additives (LMPMPs) to enhance thermal performance and control bondline thickness (BLT) of prepared liquid metal composites as thermal interface materials (TIMs). This new material is synthesized via in-situ by introducing gallium oxide into liquid metal alloys. In our recent research, we intensively investigated thermal properties of different primary liquid metal alloys containing small amounts of metal additives, and ran extensive reliability tests including power cycling, thermal cycling, and aging tests on the synthesized LMPMPs. In this paper, the thermal properties of the synthesized LMPMPs with different liquid metal alloys are studied with reliability tests that focus on power cycling by monitoring thermal resistance of LMPMPs over time using a custom power cycler. We have found power density, BLT, and different liquid metal alloys have a significant impact on thermal properties and reliability of LMPMPs. We also conducted thermal aging tests on Cu-LMPMPs-Cu sandwich specimens at 85°C in an ambient atmosphere to study the deterioration of thermal conductivity of LMPMPs over time, measured by laser flash analyzer using the layered structure method. Highly accelerated stress test (HAST) with a profile of 110°C, 85RH%, and 264 hours was used to study the decomposition of liquid metal alloys. Thermal cycling test with a profile of -40 to 125°C was employed to investigate the pump-out of LMPMPs. It has been proven that LMPMPs have much better thermal performances than polymer-based thermal grease.