A thermosetting resin system based on bismaleimide (BMI) has been developed via copolymerization with 4,4′-diaminodiphenylsulfone in the presence of a newly synthesized graphene oxide, modified using allylated siloxane (AS-GO). The curing behavior of the AS-GO-containing resin system was evaluated using curing kinetics. The dispersibility of AS-GO in the resin was observed through polarizing optical microscopy (POM), which indicates that AS-GO has good dispersibility in the resin due to GO modified with allylated siloxane which has a good phase compatibility with BMI. The effect of AS-GO on the thermomechanical and mechanical properties of the cured modified resin was also studied. Results of thermogravimetric analysis indicated that the cured sample systems display a high char yield at lower concentrations of AS-GO (≤0.5 wt%) with an improved thermal stability. Using dynamic mechanical analysis, a marked increase in glass transition temperature (T_g) with increasing AS-GO content was observed. Mechanical property analyses revealed a possible effect of AS-GO as a toughener, and the results showed that an addition of 0.3% AS-GO maximized the toughness of the modified resin systems, which was confirmed by analysis of fracture surfaces.