The use of sensitive electrochemical sensors to detect biomarkers is an effective method for the early diagnosis of several neurodegenerative diseases (NDs), such as Alzheimer's disease, Parkinson's disease, Huntington's disease, amyotrophic lateral sclerosis, etc. However, the commercialization of enzyme/aptamer-based sensors is still hampered owing to the historic drawbacks of biorecognition elements including high cost, poor stability, and complex integration technology. Non-enzymatic electrochemical sensors are more attractive compared to their traditional counterparts and can be widely harnessed owing to their low cost, high stability, sensitivity, and ease of miniaturization. This review summarizes recent research progress focusing on the construction of non-enzymatic electrochemical sensors and analyzes their present use in the early diagnosis of NDs. Additionally, this review addresses the limitations and challenges of the use of current non-enzymatic electrochemical sensor technologies for the diagnosis of NDs and highlights the possible directions for future research.