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M n+X zeolites (M n+ = Ni2+ and/or Cr3+) were prepared and characterized by various techniques. The adsorption of propylene and propane onto these zeolites was investigated, and thermodynamic properties were discussed. The objective is to establish a comparison between the binary (introduction of Ni2+ or Cr3+ instead of Na+) and ternary (introduction of Ni2+ and Cr3+ instead of Na+) exchanges. To our knowledge, there is no work in this field, in spite of a growing interest in bimetallic zeolites. Isotherms of C3H6 and C3H8 were successfully modeled using the Toth equation. A change in K H, Henry’s law slope, confirms the strong and weak characters of the interactions with propylene and propane, respectively. CrNi(39)­X has an intermediary behavior between Cr(39)­X and Ni(40)­X. It manifests specific interaction with C3H6 molecules through the deep implication of Cr3+ cations, at low coverage. With increasing adsorbate concentration, the contribution of Ni2+ occurs.