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The sustainable management of olive wastes represents an important environmental challenge. Biochars and hydrochars derived from biomass are promising adsorbents for removing emerging pollutants from water. In the present work, olive stone wastes were converted into biochar and hydrochar by using pyrolysis (500 °C for 30 min) and hydrothermal carbonization (HTC) processes (220 °C for 10 h). Then, the obtained materials were physically activated by using CO2 gas (750 °C for 30, 60 and 180 min). Various analytical techniques were applied for the chemical, textural and structural characterization of these carbonaceous materials (i.e., ultimate and proximate analysis, scanning electron microscopy (SEM), BET surface area, Raman spectroscopy, X-ray diffraction, and Fourier transform infrared spectroscopy). Afterwards, the selected activated biochar and hydrochar were applied for the removal of amoxicillin from aqueous solutions. The experimental results show that the generated hydrochar has many microspheres on its surface and inside, while the produced biochar exhibits a porous structure with irregular forms. CO2 physical activation has induced an important improvement of the biochar and hydrochar’s structural, textural, and surface chemistry properties. For instance, the activated biochar samples show a highly porous structure, with large specific surface areas that increase with the burn-off, reaching 1349.3 m2 g−1 following 3 h of activation. Regarding the activated hydrochar samples, they exhibit a spherical morphological structure with an important specific surface area, which increased to 846.7 m2 g−1 after 3 h of activation. Moreover, both activated materials have an amorphous structure with low oxygen surface groups. The selected novel CO2-activated biochar and hydrochar efficiently remove amoxicillin from aqueous solutions under wide experimental conditions, with adsorption capacities of 386.4 and 215.9 mg g−1, respectively. These efficiencies are higher than those reported for various activated biochars derived from lignocellulosic biomass, from sewage sludge, and from animal manure. Future research works are required to assess these materials’ effectiveness in treating real pharmaceutical effluents, to optimize the regeneration of the amoxicillin-loaded materials, and to design full-scale devices for a real application.