Neurological diseases like Alzheimer’s disease, epilepsy, and Parkinson’s disease pose difficult therapeutic challenges. Phytochemicals obtained from medicinal plants provide promising neuroprotective potential via anti-inflammatory, antioxidant, and neurotransmitter-modulating mechanisms. This chapter explores the integration of phytochemistry with computational drug discovery to identify and optimize plant-derived neurotherapeutic agents. Key phytochemical classes, including flavonoids, alkaloids, polyphenols, and carotenoids, are discussed for their molecular roles in modulating neuroinflammation, oxidative stress, and pathological protein aggregation. Emphasis is placed on in silico methods, for example, virtual screening, molecular dynamics simulations, molecular docking, quantitative structure-activity relationship modeling, pharmacophore modeling, and network pharmacology. Case studies are presented to illustrate phytochemicals with strong binding affinity to neurological targets, favorable interaction profiles, and potential for Multi-target function. The chapter also addresses the challenges in translating phytochemical research into clinical applications, focusing on issues such as standardization, pharmacokinetics, bioavailability, and safety. By combining computational and pharmacological perspectives, this work highlights the therapeutic promise of phytochemicals and supports their further development as innovative agents for managing complex neural disorders.