Despite the lack of substantial evidence for improvement in the quality of teaching and learning with information and communication technology (ICT), governmental organizations, including those of Canada and Australia, have made large investments into ICT. This investment has been largely predicated on the hypothesized relationship between ICT and science achievement, and the need for ICT as a means of providing broad-scale training to meet the demand for a skilled workforce. To better understand this possible relationship, this study used data from the 2006 administration of the Programme for International Student Assessment (PISA 2006) to determine the extent to which scientific literacy is predicted by student- and school-level variables related to ICT, after adjusting for student demographic characteristics and school characteristics. The findings suggest that, once student demographic characteristics and school characteristics have been accounted for, students with prior experience with ICT, who browse the Internet more frequently, and who are confident with basic ICT tasks earned higher scientific literacy scores. Gender differences existed with respect to types of productivity and entertainment software used; this difference may be attributed to personal choice and initiative to learn ICT. Finally, differences in ICT use between Canada and Australia, particularly with school use, may be due to initiatives in Australia (e.g., National Goals of Schooling for the Twenty-first Century) that promote the increased use of ICT in classrooms.