A cocuring agent is necessary for tetrafluoroethylene–propylene elastomer (FEPM), which cannot be cured by peroxide alone. We observed that high‐vinyl polybutadiene rubber (HVBR) could be used as a cocuring agent for FEPM. The structure and properties of FEPM–HVBR blend vulcanizates were investigated by 13C‐NMR, differential scanning calorimetry, swelling tests, tensile tests, dynamic mechanical analysis, and thermogravimetric analysis. This research showed that HVBR significantly improved FEPM by conferring a high crosslink degree to the FEPM–HVBR blends. When the HVBR concentration was 25% without any filler reinforcement, the tensile strength of the FEPM–HVBR blend vulcanizate reached 11.6 MPa, and the crosslinking density reached 171 μmol/cm3. In addition, HVBR improved the thermal stability of FEPM and changed the glass‐transition temperature (T
g) of the blend; as the HVBR content increased, the T
g of the blend also increased. 13C‐NMR analysis confirmed that crosslinks existed between the HVBR and FEPM macromolecules. When the blends contained trace amounts of HVBR, free‐radical reaction was more preferred between FEPM and HVBR, whereas when HVBR was 15% or more, crosslinking between HVBR was predominant. These findings expand the choices for the curing of FEPM. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 136, 47836.