A virtual learning environment (VLE) is a web-based platform that allows students to learn at a personally defined place, time and pace. However, most students are lacking in the self-regulation skills and metacognitive abilities to take advantage of the flexibility and high learners' control available in VLEs. The purpose of the study was to investigate the influence of self-regulation processes on secondary school students' metacognition within a partial least square (PLS) framework. The sample consisted of 506 secondary school students. The data analysis was run using Smart PLS Version 3.0. The results revealed that self-efficacy and procrastination were significantly related to strategy use, which in turn influenced students' metacognition. Self-efficacy was found to be the primary motivational belief that drives students' help-seeking behaviour as well as the application of task strategies and time management. The findings may help to design more effective pedagogical practices to increase metacognitive abilities among secondary school students in technologically enhanced learning environments.