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This study validated a scale of students' learning satisfaction (SLS) and self-regulated learning (SRL) strategies in MOOCs to measure the relationship between SRL and SLS based on Zimmerman's SRL theory and Piccoli's web-based Virtual Learning Environment (VLE) effectiveness theory. The process of developing the scale included literatures review, face and content validity, pilot study, data collection, and data analysis. An online self-reporting questionnaire was designed to include constructs such as goal setting (GS), task strategy (TS), self-evaluation (SE), help-seeking (HS), environment structuring (ES), time management (TM) and students' satisfaction (SA). All these constructs were assessed on a 5-point Likert scale. The data was collected from 333 Malaysian students in higher education, and it was analysed by using Partial Least Squares Structural Equation Modelling (PLS-SEM) technique. The resultant constructs have shown empirical result of good reliability and validity where the coefficients of Cronbach's alpha were ranged between 0.784 to 0.877, HTMT values were passed of 0.90 tests and factors loading were more than 0.7. The resulting constructs can be used by the practitioners, academicians, researchers, and policy makers to have a clear understanding on SLS and SRL in MOOC so that, a suitable, effective, positive, and meaningful MOOC learning environment could be established in the universities, higher education learning institutions and/or training organizations.