Drawing on the Programme for International Student Assessment 2003 data set comprising over 190,000 15-year-old students in 25 countries, the current study sought to examine the role of arts-related information and communication technology (ICT) use in students' problem-solving skill and science and mathematics achievement. Structural equation modeling indicated that the quality of arts-related ICT use positively predicted problem-solving skill, whereas the quantity of arts-related ICT use negatively predicted problem-solving skill. Importantly, however, there was an interaction between quality and quantity of ICT use such that the detrimental effect of the frequency of arts-related ICT use was more pronounced among students with low-quality ICT use than for those with high- and moderate quality ICT use. Analyses also showed that the effects of arts-related ICT use on achievement were primarily mediated by problem-solving skill. Findings hold educational implications for practitioners, policy makers, and researchers seeking to optimize the cognitive and academic benefits of ICT in the arts and the school more broadly.