Humans exhibit complex mathematical skills attributed to the exceptional enlargement of neocortical regions throughout evolution. In the current work, we initiated a novel exploration of the ancient subcortical neural network essential for mathematical cognition. Using a neuropsychological approach, we report that degeneration of two subcortical structures, the cerebellum and basal ganglia, impairs performance in symbolic arithmetic. We identify distinct computational impairments in male and female participants with cerebellar degeneration (CD) or Parkinson's disease (PD). The CD group exhibited a disproportionate cost when the arithmetic sum increased, suggesting that the cerebellum is critical for iterative procedures required for calculations. The PD group showed a disproportionate cost for equations with increasing addends, suggesting that the basal ganglia are critical for chaining multiple operations. In Experiment 2, the two patient groups exhibited intact practice gains for repeated equations at odds with an alternative hypothesis that these impairments were related to memory retrieval. Notably, we discuss how the counting and chaining operations relate to cerebellar and basal ganglia function in other task domains (e.g., motor processes). Overall, we provide a novel perspective on how the cerebellum and basal ganglia contribute to symbolic arithmetic. Our studies demonstrate the constraints on the computational role of two subcortical regions in higher cognition.Significance StatementResearch on the neurobiology of mathematics has focused on the cerebral cortex, particularly the frontoparietal regions. In the present study, we asked how disorders primarily affecting subcortical structures impact performance on symbolic arithmetic operations. Participants with Parkinson's disease showed a greater impairment as the number of operations increased, and participants with cerebellar degeneration showed a greater impairment as the magnitude of the operations increased. This selective impairment points to the distinctive roles of the cerebellum and basal ganglia in symbolic arithmetic. These results suggest that two major subcortical structures can support symbolic complex cognition.