The large number of tires produced annually demands new recycling methods. A key challenge associated with recycling elastomers is their crosslinking structure that prevents fusion. It is possible to reverse crosslinking through a process called devulcanization. Devulcanized elastomers can be blended with fresh rubber and revulcanized for reuse. This paper examines samples made from natural rubber (NR), styrene–butadiene rubber (SBR), and nitrile butadiene rubber (NBR), blended with varying proportions of devulcanized ground tire rubber (dGTR) and newly revulcanized rubber. SiO2, commonly present in tire formulations, is also added. Samples of these materials, with 0, 10, 20, and 40 phr of dGTR are subjected to accelerated degradation for 0, 30, 60, 120, and 240 h. The effects of this treatment, the influence of SiO2, and the presence of a silane-based devulcanization agent (TESPT) that promotes the interaction between the rubber and silica, are analyzed at the microstructural level (FTIR, TGA, SEM) and through mechanical properties testing. The microstructural results of the spectroscopy and thermal analysis show that interactions between dGTR, silica, and silane compounds form aggregates that impact the material properties and degradation of the tires. Mechanically, when the sample contained up to 20 phr of dGTR, the compound presented a more brittle behavior, due to the crosslinking induced by the degradation