This study explores the relationship between out-of-home behavior and daily mood of community-dwelling older adults with different levels of cognitive impairment across four consecutive weeks. The sample included 16 persons with early stage Alzheimer’s disease (AD), 30 persons with mild cognitive impairment (MCI), and 95 cognitively healthy persons (CH). Using a multi-method approach, GPS tracking and daily-diary data were combined on a day-to-day basis. AD and MCI adults showed lower mood than the CH group. Whereas stronger positive links between mood and out-of-home behavior were found for AD compared to the total sample on an aggregate level, predicting daily mood by person (i.e., cognition) and occasion-specific characteristics (i.e., mobility and weekday), using multilevel regression analysis revealed no corresponding effect. In conclusion, cognitive status in old age appears to impact on mobility and mood as such, rather than on the mood and out-of-home behavior connection.