The problem extent of the large concentration of fluoride ions in drinking water is still a central health issue. In the present study, lanthanum doped magnetic Teff straw biochar (LDMTSB) was developed as a novel adsorbent for removing fluoride ions in the groundwater in Rift-Valley regions, especially Hawassa city, Ethiopia. The synthesized LDMTBC was characterized via FTIR, XRD, SEM, and BET. And, this analysis proposed that multiadsorption techniques such as ligand exchange, precipitations, and electrostatic interaction could be evinced throughout the fluoride ions adsorption process by LDMTSB. The constraints that influence the adsorption efficacy, namely, a dosage of LDMTSB, contact time, pH of the solution, and rotational speed, were analyzed and optimized using the response surface methodology approach. Under the optimum situations, LDMTSB dosage: 3.97 g, contact time: 56.36 min, rotational speed: 591.19 rpm, and pH: 3.968 demonstrate high efficacy of LDMTSB with 98.89% fluoride removal capacity. Further, the quadratic model (R2 = 0.9841) was designated for governing the mathematical process. The LDMTSB was successful in the removal of fluoride ions in the groundwater. This study provides a valuable economical solution for the application of Teff straw.