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Neuropsychiatric disorders are of great health concerns, and despite the availability of drugs, effective therapies are poor, emphasizing the need for novel therapeutics. Among the natural substances screened for neuromodulation properties, Spirulina platensis, a cyanobacterium, and its main bioactive compound (phycocyanin) have attracted great attention. Substantial evidence demonstrates that spirulina and phycocyanin possess neuroprotective properties by targeting multiple interconnected cellular and molecular pathways, including apoptosis, oxidative stress, neuroinflammation, and regulators of synaptic plasticity. Consequently, these compounds have shown therapeutic potential in experimental models of Alzheimer's disease, Parkinson's disease, multiple sclerosis, cerebral ischemia, epilepsy, schizophrenia, depression, and autism spectrum disorder. Herein, we summarize various cellular and molecular pathways which are affected by spirulina and phycocyanin in neuropsychiatric disorders.