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Accurate assessment of physical activity (PA) is crucial in interventions promoting it and in studies exploring its association with health status. Currently, there is a wide range of assessment tools available, including subjective and objective measures. This study compared accelerometer-based estimates of PA with self-report PA data in older adults. Additionally, the associations between PA and health outcomes and PA profiles were analyzed. Participants (n = 110) wore a Xiaomi Mi Band 2® for fifteen consecutive days. Self-reported PA was assessed using the International Physical Activity Questionnaire (IPAQ) and the Yale Physical Activity Survey (YPAS). The Spearman correlation coefficient was used to compare self-reported and accelerometer-measured PA and associations between PA and health. Bland–Altman plots were performed to assess the agreement between methods. Results highlight a large variation between self-reported and Xiaomi Mi Band 2® estimates, with poor general agreement. The highest difference was found for sedentary time. Low positive correlations were observed for IPAQ estimates (sedentary, vigorous, and total PA) and moderate for YPAS vigorous estimates. Finally, self-reported and objectively measured PA associated differently with health outcomes. Summarily, although accelerometry has the advantage of being an accurate method, self-report questionnaires could provide valuable information about the context of the activity.