Perceived usefulness and perceived ease of use constitute important belief factors when technology adoption decisions are made within a non-mandatory setting. This paper investigated the role played by psychological ownership in shaping teachers' beliefs about using a cloud-based virtual learning environment (VLE). Psychological ownership is increasingly becoming a relevant phenomenon in technology adoption research, where people can feel psychologically attached to a particular technology. The study proposed that such phenomenon can also occur when using a VLE, and a hypothesised model with six constructs was tested with 629 Malaysian teachers from 21 schools. Results from structural equation modelling-partial least squares analysis found teachers' experiences with the VLE significantly influenced psychological ownership, which in turn significantly predicted perceived usefulness and perceived ease of use of the VLE. Overall, the model possesses predictive relevance for the outcome predictors as indicated by Stone-Geisser's , and accounted for 61.6% of variance in perceived usefulness and 62.0% of variance in perceived ease of use. This study provides insights into the motivation behind teachers' beliefs which are shaped by their experiences with the VLE. Implications for theory and practice were discussed based on the insights of the study.