This paper presents a low-cost, high-temperature-resistant and high-strength polyacrylamide gel system formed by secondary cross-linking. The gel system (named JM186) used phenolic resin and organic zirconium as cross-linking agents, and the performance of the gel system was systematically evaluated under high temperature. The gel properties studied include: gel formation time, gel strength, thermal stability, sand-filled pipe sealing efficiency, and its microstructure. The concentration of polyacrylamide in JM186 gel system was as low as 0.3%, which can control the gelling time in a range of 1–9 h by adjusting the ratio of two cross-linking agents. It can resist temperature up to 120 °C without dehydration, and its highest gel strength can reach H grade. The modulus of elasticity (G’) and viscosity (G”) can reach 32.33 Pa and 3.25 Pa, respectively. DSC (differential scanning calorimetry) test indicated that the temperature of structural failure for this composite gel is 310.5 °C. The average sealing efficiency of the gel is 96.03% in sand-filled pipes. Finally, the gel microstructure was observed by cryo-scanning electron microscopy (Cryo-SEM). It was found that the gel system by secondary cross-linking has a dense and thickened network structure compared with the single cross-linker gel system. The gel is cross-linked by both the coordination bond and covalent bond, and the two cross-linking agents have a synergistic effect. This is the reason why the secondary cross-link gel system is better than the single-cross-linker gel system.