A converging body of evidence from neuroimaging, behavioral, and neuropsychology studies suggests that different arithmetic operations rely on distinct neuro-cognitive processes: while addition and subtraction may rely more on visuospatial reasoning, multiplication would depend more on verbal abilities. In this paper, we tested this hypothesis in a longitudinal study measuring language and visuospatial skills in 358 preschoolers, and testing their mental calculation skills at the beginning of middle school. Language skills at 5.5 years significantly predicted multiplication, but not addition nor subtraction scores at 11.5 years. Conversely, early visuospatial skills predicted addition and subtraction, but not multiplication scores. These results provide strong support for the existence of a double dissociation in mental arithmetic operations, and demonstrate the existence of long-lasting links between language/visuospatial skills and specific calculation abilities.