Boron is an essential element for plants and living organisms; however, it can be harmful if its concentration in the environment is too high. In this paper, lanthanum(III) ions were introduced to the structure of chitosan via an encapsulation technique and the obtained hydrogel (La-CTS) was used for the elimination of the excess of B(III) from modelling solutions. The reaction between boric acid and hydroxyl groups bound to the lanthanum coordinated by chitosan active centres was the preponderant mechanism of the bio-adsorption removal process. The results demonstrated that La-CTS removed boric acid from the aqueous solution more efficiently than either lanthanum hydroxide or native chitosan hydrogel, respectively. When the initial boron concentration was 100 mg/dm3, the maximum adsorption capacity of 11.1 ± 0.3 mg/g was achieved at pH 5 and the adsorption time of 24 h. The successful introduction of La(III) ions to the chitosan backbone was confirmed by Scanning Electron Microscopy with Energy Dispersive X-Ray Spectroscopy, Fourier-Transform Infrared Spectroscopy, X-Ray Diffraction, X-ray Photoelectron Spectroscopy, and Inductively Coupled Plasma Optical Emission Spectroscopy. Due to its high-performance boron adsorption-desorption cycle and convenient form, La-CTS seems to be a promising bio-adsorbent for water treatment.