Amyotrophic lateral sclerosis (ALS) is the most common adult-onset motor neuron disease, characterized by rapid loss of upper and lower motor neurons resulting in patient death from respiratory failure within 3-5 years of initial symptom onset. Although at least 30 genes of major effect have been reported, the pathobiology of ALS is not well understood. Compounding this is the lack of a reliable laboratory test which can accurately diagnose this rapidly deteriorating disease. This barrier has created a severe road-block for researchers trying to develop novel therapeutics and clinicians initiating treatments. Therefore, alongside identification of etiologies and therapeutics, development of a diagnostic and prognostic biomarker is a foremost research priority. Herein, we report the use of graphene, a sensitive nanomaterial, in combination with Raman spectroscopy to identify specific signals in the cerebrospinal fluids (CSF) of ALS patients which in the future can be used to develop a diagnostic biomarker. We demonstrate that the second-order overtone of in-plane phonon vibration energies (2D) of interfaced graphene can be sensitively modified by the components in the CSF. The n-doping mechanism employed by our platform is disease specific, with a 2D vibration energy shift of approximately 3.3±0.3 cm-1 in the case of ALS patients.