Most studies on enhanced polymer gels look at modifying the interaction between the polymer matrix and fillers. Here, a new strategy is proposed for the fabrication of a new kind of polyacrylamide/Ca(OH) nanocomposite organogel with tunable mechanical properties and temperature tolerance. By changing the solvent component, the properties of an organogel can be modulated without adding further reinforcing agent. Two commonly used organic solvents, glycerin (GL) and ethylene glycol (EG), were used in different weight ratios (GL:EG = 100:0, 70:30, 50:50, 30:70, 0:100) to achieve modulation of the organogel properties. At 25 °C the compressive strength could be regulated in the range 18–29 MPa at 95% strain, and it could be kept in the range 12–46 MPa within the temperature range −25 °C–110 °C. Increasing the proportion of GL, which has a high boiling point, the high and low temperature tolerance of the organogel was strengthened significantly. The EG served as a lubricant and enhanced the tensile recoverability from 77% to 84%. Overall, the properties of the organogel were the best when the GL:EG ratio was 70:30. The solvent-switchable organogel fabricated in this study is a good candidate for extending the field of application of gel materials.