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The present study aims to examine the structural relationships between pre-service teachers’ information and communication technology (ICT) competences, including basic ICT literacy, learning skills with ICT, and teaching skills with ICT. About fourteen thousand pre-service teachers from 14 normal universities in 11 provinces in China participate in this study. Using structural equation modeling, the present study reveals that basic ICT literacy, specifically in terms of mastery of technical environments, strongly predict learning and teaching skills with ICT. Learning skills with ICT, specifically in the domain of research and innovating with ICT, mediate the relationships between basic ICT literacy and teaching skills with ICT. The present study highlights the importance of learning skills with ICT in pre-service teacher education programs.