In this study, cooperative bifunctional materials (BFMs)�composed of combined adsorbent and catalyst materials� are synthesized and processed through additive manufacturing by 3D printing adsorbent/catalyst monoliths with a CaO adsorbent phase balanced against an M@ZSM-5 (M = In, Ce, Cr, or Mo oxide) heterogeneous catalyst phase. The adsorbent/catalyst monoliths were characterized using NH 3 -TPD, H 2 -TPR, N 2 physisorption, X-ray photoelectron spectroscopy, X-ray diffraction, pyridine-Fourier transform infrared spectroscopy, C 3 H 8 -diffuse reflectance infrared Fourier transform spectroscopy, and energydispersive spectroscopy. Their performances were evaluated for combined CO 2 capture and propane dehydrogenation at 600−700 °C. These experiments revealed that a reaction temperature of 600 °C generates the best performance for all samples due to the shift toward thermal cracking at higher temperatures. Moreover, 600 °C was usable for both CO 2 adsorption and catalysis, so the materials reported here could truly perform both adsorption and catalysis isothermally. Of the materials, CaO-Mo@ZSM-5 displayed the best performance, generating 20.4% propylene yield, 20% propane conversion, 75% CO 2 conversion, and 5.4 mmol/g CO 2 capture capacity at 600 °C. The stability of this sample was then assessed across ten adsorption/reaction cycles at T = 600 °C, where its propane conversion, CO 2 conversion, and propylene yield varied by less than 5% across the entirety of the experiment. Overall, this work accomplishes three key goals: it (i) expands the concept of BFM materials to a previously unexplored reaction for direct CO 2 capture from air (direct air capture) or flue gas, and subsequent utilization, (ii) provides a facile way of structuring BFM materials into practical contactors, and (iii) allows adsorption and catalysis to occur at the same temperature with high cyclic stability within a single bed.