Scientific collaboration between neuroscience and mathematics education has mostly focused on brain imaging trying to inform education. This study aims at meeting expectations of both research fields, thus enhancing the ecological validity. We investigated the influence of age, mathematical competency, and task characteristics (format, complexity) on students' arithmetic performance. Based on behavioral data from a pilot study (n = 73), arithmetic tasks were chosen for a subsequent investigation (n = 90), in which parietal brain activation was measured with near-infrared spectroscopy. Substantial group differences in calculation time were observed. While task characteristics influenced arithmetic performance in both age groups, this influence was much smaller for grade 8 students. However, parietal brain activation during calculation was not affected by age, mathematical competency, or task characteristics. Limitations of the experimental design and general problems of applying imaging methods to the school context are discussed.