Different aspects of second-language learners’ autonomous use of technology for language learning have been investigated and its positive effects on language learning have been reported. However, there is a paucity of research on whether language learners’ different proficiency levels are associated with their perceptions of their own autonomous use of technology-enhanced language learning (TELL). Therefore, this study examines the autonomous use of TELL outside the English classes of English learners of different proficiency levels. Ninety-nine EFL college students (47 of lower proficiency and 52 of higher proficiency) in northern Taiwan took a survey on the autonomous use of TELL. The results demonstrated that students’ proficiency levels did not relate to the involvement of autonomous use of technology for language learning. Nearly one-third of all students did not take on autonomous English learning via technology outside class. The students in both groups tended towards more receptive-skill English learning activities than productive-skill activities in their autonomous use of technology, whereas the students of higher proficiency attended more productive-skill activities than those of lower proficiency. In order for students to benefit from the autonomous use of technology for language learning, proper support and guidance from instructors are crucial.