A growing body of research has examined the relations of dispositions toward information and communication technology (ICT) to science achievement among adolescent students. However, there is little research exploring the associations between ICT-related dispositions and science-related dispositions among adolescent students. Therefore, this study, employing a self-determination theory perspective, investigated the relationships of perceived competence in ICT usage and perceived autonomy related to ICT usage with dispositions toward science-enjoyment of science, interest in broad science topics, science self-efficacy, and epistemological beliefs about science-among 258,192 adolescent students from 10,767 schools in 42 PISA 2015 participating countries. Results of multilevel structural equation modeling (MSEM) analyses, after accounting for student-, school-, and country-level demographic characteristics, indicated that students' perceived competence in ICT usage and perceived autonomy related to ICT usage were significantly positively related to their enjoyment of science, interest in broad science topics, science self-efficacy, and epistemological beliefs about science. Further, the results of the study revealed that students' perceived autonomy related to ICT usage was more strongly associated with their dispositions toward science than perceived competence in ICT usage. Implications of the findings for policy and practice are discussed.