The main purpose of this paper is to bring pioneering insights into the core line of sustainable education research by investigating the multi-dimensional aspects of teachers’ readiness to design technology-enhanced learning environments. In order to achieve this goal, this study documents the experiences of pre-service English teachers in instructional Virtual Reality (herein, VR) content design of K–12 English digital textbooks. Furthermore, it examines how their VR creation can be linked to a metaverse platform for learning adaptivity and sustainable education. The data are collected by pre-/post-surveys as well as reflective papers. The pre-/post-survey responses are analyzed with a t-test to determine significance; the reflective paper entries are scrutinized with sentiment analysis and text mining. The study findings suggest that such transformative experiences of VR-Making (herein, VRM) for instructional contents are conducive to capacitate pre-service teachers’ technological readiness, 4Cs (Critical Thinking, Creativity, Collaboration, Communication) in digital citizenship, and perceived pedagogical benefits. Based on findings, this study continues to support the need for providing teaching practitioners with hands-on learning-to-teach opportunities with emerging technology as a tool to fulfill sustainable education.