In the present study, polychloroprene (CR) compounds containing different vulcanization agents and fumed silica at varied content are evaluated for application as adhesives. The vulcanization systems are based on zinc oxide (ZnO) or ferric acetylacetonate (FeAc). The fumed silica content varied from 0.3 up to 2.0 phr only in CR–FeAc compounds. The rheometric results indicated that the CR compounds containing FeAc reached a higher crosslink density, ≈ 1.5 higher than that observed for the CR compound vulcanized with the ZnO system. After vulcanization, the CR–ZnO compound shows the highest tensile strength and elongation at break. In the T‐Peel tests, in which different solvents are tested in the unvulcanized CR compounds, the compositions containing ZnO in toluene/methyl ethyl ketone (MEK) show the highest adhesive strength. Among the CR–FeAc compounds, the addition of 2 phr of fumed silica results in the highest tensile strength and elongation at break, while the compound containing 1 phr of fumed silica shows the highest adhesive strength.