Background Although healthy aging can be stimulated by the reduction of sedentary behavior, few interventions are available for older adults. Previous studies suggest that self-monitoring might be a promising behavior change technique to reduce older adults’ sedentary behavior. However, little is known about older adults’ experiences with a self-monitoring–based intervention aimed at the reduction of sedentary behavior. Objective The aim of this study is to evaluate engagement, acceptability, usability, and preliminary efficacy of a self-monitoring–based mHealth intervention developed to reduce older adults’ sedentary behavior. Methods A mixed methods study was performed among 28 community-dwelling older adults living in Flanders, Belgium. The 3-week intervention consisted of general sedentary behavior information as well as visual and tactile feedback on participants’ sedentary behavior. Semistructured interviews were conducted to explore engagement with, and acceptability and usability of, the intervention. Sitting time was measured using the thigh-worn activPAL (PAL Technologies) accelerometer before and after the intervention. System usage data of the app were recorded. Quantitative data were analyzed using descriptive statistics and paired-samples t tests; qualitative data were thematically analyzed and presented using pen profiles. Results Participants mainly reported positive feelings regarding the intervention, referring to it as motivating, surprising, and interesting. They commonly reported that the intervention changed their thinking (ie, they became more aware of their sedentary behavior) but not their actual behavior. There were mixed opinions on the kind of feedback (ie, tactile vs visual) that they preferred. The intervention was considered easy to use, and the design was described as clear. Some problems were noticed regarding attaching and wearing the self-monitoring device. System usage data showed that the median frequency of consulting the app widely differed among participants, ranging from 0 to 20 times a day. No significant reductions were found in objectively measured sitting time. Conclusions Although the intervention was well perceived by the majority of older adults, no reductions in sitting time were found. Possible explanations for the lack of reductions might be the short intervention duration or the fact that only bringing the habitual sedentary behavior into conscious awareness might not be sufficient to achieve behavior change. Trial Registration ClinicalTrials.gov NCT04003324; https://tinyurl.com/y2p4g8hx