Global carbon dioxide emissions are rising and the use of fossil fuels in several sectors are the leading causes. As global population and economies continue to grow significantly, the most practical method of lowering such emissions is to capture CO2. Although other technologies are more developed, adsorption is very promising and has attracted much attention. To ensure this technology’s success, it is essential to have suitable CO2 adsorbent materials. In this work, several new hydrotalcites (HTs) with different initial concentrations of ion precursors were prepared for the first time by the co-precipitation method—it was possible to verify that the ion concentrations influence the characteristics of the materials. The prepared HTs were characterized by thermogravimetric analysis (TG), X-Ray diffraction (XRD), surface area measurements and temperature-programmed desorption of CO2 (TPD-CO2) to relate their CO2 capture capacity to their physicochemical properties; the CO2 adsorption equilibrium isotherms were determined at 35 and 300 °C for the prepared samples, as well as for some commercial materials: magnesium oxide, calcium oxide, aluminium oxide and Zeolite 13X. After determining which materials present the best CO2 adsorption capacity, these were submitted to adsorption-desorption cycles to study their stability. The main objective of the work was to prepare and study different CO2 adsorbents for processes that are carried out at low and intermediate temperatures. From the experimental results, it was possible to conclude that the Zeolite 13X showed the best capacity at 35 °C, 3.38 mmol·g−1 (@ pCO2 = 1 bar), and a prepared calcined HT (c-HT2) was the best at 300 °C, 0.97 mmol·g−1 (@ pCO2 = 1 bar). Moreover, it seems there is an optimum initial concentration of the ions’ solutions for the tested HTs, which depends on the final application—c-HT1 showed a better capacity at 35 °C and c-HT2 at 300 °C. From the adsorption-desorption cycles—performed at 35 and 300 °C with the best materials using a magnetic suspension microbalance at 1 bar of CO2 partial pressure —, a working cyclic capacity of 2.69 mmol∙g−1 was achieved by the Zeolite at 35 °C; in turn, c-HT2 showed a working cyclic capacity of 0.79 mmol∙g−1 at 300 °C.