This article reports the development and validation of an instrument, the Technology-Based Self-Regulated English Learning Strategies Scale (TSELSS), in terms of its multifaceted structure of self-directed use of technology in English learning among Chinese university EFL students. TSELSS was developed through a three-phase process, focusing on the domain of self-regulated English learning in technology-assisted conditions. The first phase involved the generation of an item pool, the second a pilot study (N = 164) aimed at identifying the factor structure of TSELSS using exploratory factor analysis, and the third an examination of the psychometric properties of the revised TSELSS using confirmatory factor analysis with another independent sample of students (N = 525). Furthermore, the concurrent validity of TSELSS was investigated through correlations with students’ English language self-efficacy and English learning outcomes. The final version of the scale is made up of five types of technology-based self-regulated English learning strategies: motivational regulation strategies, goal setting and learning evaluation, social strategies, technology-based English song and movie learning, and technology-based vocabulary learning. The TSELSS can be used as an evaluation tool to appraise EFL students’ technology-based self-regulated English learning experience, and as a research tool to investigate more associations between technology-based self-regulated strategic English learning and other contextual and learner individual factors.