<p>Trace elements play essential roles in neural homeostasis by modulating energy metabolism, redox balance, neurotransmitter synthesis, and synaptic plasticity, processes directly related to cognition and mood. Elements such as zinc, iron, copper, selenium, iodine, and phosphorus act as enzymatic cofactors and regulators of neuronal excitability, while their imbalance has been associated with cognitive impairment, affective alterations, and increased vulnerability to neurodegenerative diseases. In contrast, heavy metals such as lead, mercury, cadmium, arsenic, aluminum, and bismuth are neurotoxic agents capable of triggering oxidative stress, neuroinflammation, mitochondrial dysfunction, and alterations in neurotransmission, thereby contributing to memory deficits, executive dysfunction, and symptoms of anxiety and depression. Given the need for methods capable of detecting early chemical alterations associated with metal dyshomeostasis, Raman spectroscopy has emerged as a promising analytical tool, as it enables the noninvasive identification of vibrational signatures related to biomolecules and metal–protein interactions in tissues and biofluids. In addition, surface-enhanced Raman spectroscopy (SERS) increases the sensitivity of the technique through metallic nanostructures, enabling detection at ultralow concentrations. The integration of Raman spectroscopy with machine learning methods has the potential to improve spectral pattern discrimination and to enable biomarkers capable of reflecting dysfunctional neurochemical states prior to clinical onset. Thus, Raman and SERS represent innovative approaches for investigating and monitoring the interface between metals, neurotoxicity, cognition, and mental health.</p>