The employment of compounds obtained from natural sources to produce adsorbents and their application in the elimination of antibiotics from industrial effluents have gained significant attention because of their low production cost and sustainability. Herein, chitosan (biopolymer) and smectite (abundant clay mineral) were used for the low-cost and eco-friendly synthesis of a new type of adsorbent. A low-energy-consumption hydrothermal process was applied to the synthesis of the chitosan-derived carbon–smectite nanocomposite with cobalt (H_Co/C-S). The produced nanocomposite was characterized using elemental analysis, ICP-OES, XRPD, low-temperature N2 adsorption–desorption isotherms, FTIR analysis, and point of zero charge. H_Co/C-S (SBET = 0.73 m2 g−1, d001 = 1.40 nm, pHPZC = 5.3) was evaluated as a ciprofloxacin adsorbent in aqueous solution. Experimental data were fitted with different kinetic models and interpreted by selected adsorption isotherms. The pseudo-second-order model was found to be the most appropriate, while ciprofloxacin adsorption onto H_Co/C-S was best described by the Redlich–Peterson isotherm (R2 = 0.985). The maximum adsorption capacity of H_Co/C-S, according to the Langmuir isotherm (R2 = 0.977), was 72.3 mg g−1. Desorption and thermodynamic studies were performed. The obtained results indicated that the new hierarchically designed H_Co/C-S has promising potential to be further tested for application in real wastewater treatment.