Adequate levels of vitamins and minerals are essential for optimal neural functioning. A high proportion of individuals, including children, suffer from deficiencies in one or more vitamins or minerals. This study investigated whether daily supplementation with vitamins/minerals could modulate cognitive performance and mood in healthy children. In this randomised, double-blind, placebo-controlled, parallel groups investigation, eighty-one healthy children aged from 8 to 14 years underwent laboratory assessments of their cognitive performance and mood pre-dose and at 1 and 3 h post-dose on the first and last days of 12 weeks' supplementation with a commercially available vitamins/mineral product (Pharmaton Kiddi™). Interim assessments were also completed at home after 4 and 8 weeks at 3 h post-dose. Each assessment comprised completion of a cognitive battery, delivered over the Internet, which included tasks assessing mood and the speed and accuracy of attention and aspects of memory (secondary, semantic and spatial working memory). The vitamin/mineral group performed more accurately on two attention tasks: ‘Arrows’ choice reaction time task at 4 and 8 weeks; ‘Arrow Flankers’ choice reaction time task at 4, 8 and 12 weeks. A single task outcome (Picture Recognition errors) evinced significant decrements at 12 weeks. Mood was not modulated in any interpretable manner. Whilst it is possible that the significant improvements following treatment were due to non-significant numerical differences in performance at baseline, these results would seem to suggest that vitamin/mineral supplementation has the potential to improve brain function in healthy children. This proposition requires further investigation.