It is important to recover La3+ from metallurgical solutions or wastewater. However, the recovery rate of La3+ is usually less than 1% and the recovery methods are not environmentally friendly or user-friendly. Therefore, a straightforward, efficient, clean, and economically friendly method is needed. In this investigation, a modified adsorbent, COSAC-Na2EDTA-15, which was made from the Camellia oleifera shell (COS) and disodium ethylenediaminetetraacetic acid (Na2EDTA), was invented. In addition, characterization of the COSAC-Na2EDTA-15 adsorbent was conducted using SEM and XPS, and the principle of adsorption was revealed. The adsorption kinetics followed P-S-O KM, while the isotherm of COS-activated carbon (COSAC) aligned more closely with the Langmuir model. Compared to COSAC, the maximum La3+ adsorption capacity of COSAC-Na2EDTA-15 increased from 50 to 162.43 mg/g, and the content of O and N changed from 7.31% and 1.48% to 12.64% and 4.15%, respectively. The surface of the COSAC-Na2EDTA-15 exhibited abundant C, N, and O elements, and La3+ was detected on the sample surface after adsorption. The test and analysis results fully indicate that La3+ can be successfully adsorbed on the surface of COSAC-Na2EDTA-15. Because of its easy preparation, low cost, and superior performance, activated carbon made from COS finds extensive applications in the adsorption and recovery of rare earth elements.