Increased exposure or elevated levels of aluminium(Al) in humans cause various detrimental pathological processes especially affecting the central nervous system. Al-induced neurotoxicity predominantly leads to impaired motor coordination, cognition and learning and memory deficits. Significant association of chronic Al exposure with several neurological disorders, including Alzheimer’s disease (AD), amyotrophic lateral sclerosis (ALS) Parkinson's disease (PD) and multiple sclerosis (MS) is evident where it instigates aberrant expression of various proteins via alterations in post-translational modifications (PTMs). In depth understanding of mechanism of action of Al, effect of altered PTMs and their detection methods is essential to revert anomalies induced by Al in these neurological disorders. The present chapter will attempt to summarize the role of Al in modulation of significant PTMs including phosphorylation, methylation, oxidation, ubiquitination and provide insights into its involvement in various neurological disorders.