In order to cure hydroxyl-terminated polybutadiene (HTPB) at room temperature, tetramethyl-terephthalobisnitrile oxide (TTNO) was synthesized from 1,2,4,5-tetramethylbenzene with four steps by bromomethylation, oxidation, condensation and dehydrogenation reactions with a total yield of 50%. Their structures were characterized by FT-IR 1H NMR and 13C NMR. Define R value equals molar ratio of –CNO and C=C. We chose 0.03, 0.04, 0.05, 0.06 and 0.07 as R value to prepare the dumbbell-shaped cross-linked polymers. The FT-IR, tensile strength, DSC, TG and contact angle of the cross-linked polymers were tested and analyzed. With the increasing of R value, tensile strength of cross-linked polymer increase from 0.201MPa to 0.512 MPa, Tg from -73.08℃ to -66.70℃ and the contact angle decrease from 98.80° to 73.54°. The results shows that tetramethyl-terephthalobisnitrile oxide can curing HTPB at 25℃, the cross-linked polymers are expected to be used in the composite solid propellant.