The extensive utilization of petrochemical energy sources has led to greenhouse gas emissions, the greenhouse effect, the frequent occurrence of extreme weather events, and the severe degradation of Earth’s ecosystems. The development of renewable energy technologies has become an inevitable trend. This paper investigates an adsorption-based cooling/heating/power generation technology driven by low-grade solar thermal energy. The research results demonstrate that the adsorption performance of vermiculite compound adsorbents impregnated with LiCl solution is superior to those impregnated with CaCl2 solution, with the former exhibiting adsorption at lower p/po partial pressure ratios. Furthermore, at an adsorption bed temperature of 25 °C and a p/po partial pressure of 0.8, the adsorption cooling performance of Comp. 2 compound adsorbent impregnated with LiCl solution reaches 5760.7 kJ/kg, with a coefficient of performance (COP) of 0.75, heating performance of 9920.8 kJ/kg, COPh of 1.51, and power generation capacity of 10.6 kJ/kg. This research contributes to the advancement of sustainable energy technologies and the mitigation of environmental impacts associated with petrochemical energy sources.