A physically active lifestyle has been related to positive health outcomes and high life expectancy, but the underlying psychological mechanisms maintaining physical activity are rarely investigated. Tremendous technological progress yielding sophisticated methodological approaches, i.e., ambulatory assessment, have recently enabled the study of these mechanisms in everyday life. In practice, accelerometers allow to continuously and objectively monitor physical activity. The combination with e-diaries makes it feasible to repeatedly assess mood states in real-time and real life and to relate them to physical activity. This state-of-the-art methodology comes with several advantages, like bypassing systematic distortions of retrospective methods, avoiding distortions seen in laboratory settings, and revealing an objective physical activity assessment. Most importantly, ambulatory assessment studies enable to analyze how physical activity and mood wax and wane within persons over time in contrast to existing studies on physical activity and mood which mostly investigated between-person associations. However, there are very few studies on how mood dimensions (i.e., feeling well, energetic and calm) drive non-exercise activity (NEA; such as climbing stairs) within persons. ... mehrRecent reviews argued that some of these studies have methodological limitations, e.g., scarcely representative samples, short study periods, physical activity assessment via self-reports, and low sampling frequencies. To overcome these limitations, we conducted an ambulatory assessment study in a community-based sample of 106 adults over one week. Participants were asked to report mood ratings on e-diaries and to wear an accelerometer in daily life. We conducted multilevel analyses to investigate whether mood predicted NEA, which was defined as the mean acceleration within the 10-minute interval directly following an e-diary assessment. Additionally, we analyzed the effects of NEA on different time frames following the e-diary prompts in an exploratory manner. Our results revealed that valence significantly and positively predicted NEA within persons (p=.001). Feeling more energetic was associated with significantly increased NEA (p<.001), whereas feeling calmer was associated with significantly decreased NEA (p<.001) on the within-person level. The analyses on different time frames of NEA largely confirmed our findings. In conclusion, we showed that mood predicted NEA within adults but with distinct magnitudes and directions of effects for each mood dimension.