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Ecological momentary assessment (EMA) is a methodological tool that can provide novel insights into the prediction and modeling of physical behavior; however, EMA has not been used to study physical activity (PA) or sedentary behavior (SB) among racial minority older adults. This study aimed to determine the feasibility and validity of an EMA protocol to assess racial minority older adults’ PA and SB. For 8 days, older adults (n = 91; 89% African American; 70% earning <$20,000/year) received six randomly prompted, smartphone-based EMA questionnaires per day and wore an activPAL monitor to measure PA and SB. The PA and SB were also self-reported through EMA. Participants were compliant with the EMA protocol on 92.4% of occasions. Participants were more likely to miss an EMA prompt in the afternoon compared to morning and on weekend days compared to weekdays. Participants were less likely to miss an EMA prompt when engaged in more device-based SB in the 30 min around the prompt. When participants self-reported PA, they engaged in less device-based PA in the 15 min after compared to the 15 min before the EMA prompt, suggesting possible reactance or disruption of PA. EMA-reported PA and SB were positively associated with device-based PA and SB in the 30 min around the EMA prompt, supporting criterion validity. Overall, the assessment of low-income, African American older adults’ PA and SB through EMA is feasible and valid, though physical behaviors may influence compliance and prompting may create reactivity.