With the rapid development of the transport industry, there is a higher demand for environmental friendliness, durability, and stability of tires. Rubber composites with excellent mechanical properties, abrasion resistance, and low heat generation are very important for the preparation of green tires. In this study, the all-aqueous phase process was initially employed to prepare 2-Amino-5-mercapto-1,3,4-thiadiazole (AZT) functionalized graphene oxide (AGO). Subsequently, modified graphene oxide/silica/natural rubber (AGO/SiO2/NR) composites were obtained through latex blending and hot press vulcanization processes. This method was environmentally friendly and exhibited high modification efficiency. Benefiting from the good dispersion of AGO in the latex and the cross-linking reaction between AGO and NR, AGO/SiO2/NR composites with good dispersion and enhanced interfacial interaction were finally obtained. AGO/SiO2/NR composites showed significantly improved overall performance. Compared to GO/SiO2/NR composites, the tensile strength (28.1 MPa) and tear strength (75.3 N/mm) of the AGO/SiO2/NR composites were significantly increased, while the heat build-up value (10.4 °C) and DIN abrasion volume (74.9 mm3) were significantly reduced. In addition, the steady-state temperature field distribution inside the tire was visualized by ANSYS finite element simulation. The maximum temperature of the prepared AGO/SiO2/NR was reduced by 18.2% compared to that of the GO/SiO2/NR tires. This strategy is expected to provide a new approach for the development of low energy consumption, environmentally friendly, and long-life rubber for tires.