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Students may use ICTs for different purposes, and differing configurations of use may have unique implications for computer and information literacy (CIL); however, only few studies have directly examined how students simultaneously use ICTs across multiple domains and how such differential use configurations are related to CIL achievement. Adopting a multidimensional person-centered approach, we examined students’ (N = 5309) ICT use profiles and their relations with CIL achievement. Additionally, we investigated ICT self-efficacy and interest, gender, and SES as predictors of ICT use profile membership. Results revealed four ICT-use profiles (Academic-Use Dominant; Weak Social-Use Dominant; Low ICT Use; High ICT Use). CIL achievement was found to significantly differ across the profiles, and self-efficacy, interest, gender, and SES predicted profile membership.