The use of virtual learning environments (VLE) has grown exponentially in the past years. Research indicates that students’ online learning behavior predicts their academic performance and that students’ academic emotions can play a key role in this process. However, few studies have attempted to investigate the effectiveness of VLE activities in learning achievement within psychology education. In this longitudinal study, we analyzed the relationship between students’ activity in a VLE, their attendance, academic emotions, and module grades at a face-to-face-based university in the United Kingdom. Data were collected over 1 year across two research methods modules, each of which is compulsory for a psychology degree. VLE and attendance data from 210 students were gathered for the first-year module, with 152 students continuing to the second year. The data were cross-referenced with students’ module grades, alongside self-reported emotion data for a subset of students. The results showed that overall VLE activity and the use of specific online tools such as optional online tests and lecture recording were important predictors of academic achievement. While some significant relationships between emotions and student’s learning behavior and achievement were found, these correlations were relatively small and not consistent throughout the year. These findings have potential implications for curriculum design, particularly by making psychology educators aware of the usefulness of VLE activities and tools from the onset of students’ research methods learning journey.