Recent evidence documents the negative impact of obesity, diabetes mellitus, and other metabolic dysregulation on neurocognitive function. This review highlights a key dietary factor in these relationships: refined carbohydrates. Chronic consumption of refined carbohydrates has been linked to relative neurocognitive deficits across the lifespan. Hippocampal function is especially impacted, but prefrontal and mesolimbic reward pathways may also be altered. Early life exposure to refined carbohydrates, (i.e., prenatal, juvenile, and adolescence periods) may be particularly toxic to cognitive functioning. The impact of acute carbohydrate administration is mixed, with some findings showing benefits while others are neutral or negative. Potential mechanisms of the carbohydrate-cognition relationship include dysregulation in metabolic, inflammatory, and vascular factors, whereas moderators include age, genetic factors, physiological (e.g., glucoregulatory) function and the timing and type of carbohydrate exposure. Critically, the negative neurocognitive impacts of diets high in refined carbohydrates have been shown to be independent of total body weight. Neurocognitive deficits induced by a diet high in refined carbohydrates may manifest before overt obesity or metabolic disease onset, suggesting that researchers and providers may need to target subclinical metabolic, inflammatory, and vascular dysregulation factors in efforts to preserve cognitive function across the lifespan.