Recently, natural zeolites have started to be used as alternative materials for ozone abatement from working environments. In this study, a surface response methodology based on a D-Optimal design is applied to develop a transition-metal-modified natural zeolite that increases ozone removal efficiency. Ozone adsorption and/or decomposition onto natural and cobalt modified natural zeolite were studied by diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). Results evidenced that ozone is adsorbed and decomposed at strong Lewis acidic sites, whereas ozone adsorption products interact with surface OH groups. Additionally, DRIFTS studies indicate that nitrous species are adsorbed at acidic sites, reducing the capacity to decompose ozone when ozone is generated from air.