The increasing aged-associated neurodegenerative diseases, including Alzheimer's and Parkinson's diseases, are perplexing the world due to the incurability of these diseases in the advanced stage. It is crucial to develop an early diagnosis, which can be realized by detecting an effective biomarker like neurofilament-light chains (NfL). In this research, a lanthanide-doped MOFs (La/UiO-66-NH2) material is synthesized and pyrolyzed as a precursor to obtain a novel MOFs-derived material (ZrO2@La2O3) with excellent electrochemical properties and effective immobilization of antibodies. ZrO2@La2O3 is recruited as an electrode modification material to construct a label-free electrochemical immunosensor. Under optimal incubation conditions, the immunosensor responds to NfL in a range of 0.05 ∼ 200 ng·mL−1 with a detection limit of 0.012 ng·mL−1 (S/N = 3). The excellent performance is attributed to the spatial and electronic structure of ZrO2@La2O3 obtained by doping with lanthanum (La) and pyrolysis. The fabricated immunosensor is featured with low cost, simple fabrication and rapid detection, which might be an efficient platform satisfying demand for determination of NfL in the future and significantly assists the clinical diagnosis and treatment of neurodegenerative diseases.