Older adults struggle to maintain newly initiated levels of physical activity (PA) or sedentary behavior (SB) and often regress to baseline levels over time. This is partly because health behavior theories that inform interventions rarely address how the changing contexts of daily life influence the processes regulating PA and SB or how those processes differ across the behavior change continuum. Few studies have focused on motivational processes that regulate the dynamic nature of PA and SB adoption and maintenance on microtimescales (ie, across minutes, hours, or days). The overarching goal of Project Studying Maintenance and Adoption in Real Time (SMART) is to determine the motivational processes that regulate behavioral adoption versus maintenance over microtimescales, using a dual process framework combined with ecological momentary assessment and sensor-based monitoring of behavior. This paper describes the recruitment, enrollment, data collection, and analytics protocols for Project SMART. In Project SMART, older adults engaging in at least 30 minutes of moderate-to-vigorous intensity PA per week complete 3 data collection periods over 1 year, with each data collection period lasting 14 days. Across each data collection period, participants wear an ActiGraph GT3X accelerometer (ActiGraph, LLC) on their nondominant waist and an ActivPAL micro4 accelerometer (PAL Technologies, Ltd) on their anterior thigh to measure PA and SB, respectively. Ecological momentary assessment questionnaires are randomly delivered via smartphone 10 times per day on 4 selected days in each data collection period and assess reflective processes (eg, evaluating one's efficacy and exerting self-control) and reactive processes (eg, contextual cues) within the dual process framework. At the beginning and end of each data collection period, participants complete a computer-based questionnaire to learn more about their typical motivation for PA and SB, physical and mental health, and life events over the course of the study. Recruitment and enrollment began in January 2021; enrollment in the first data collection period was completed by February 2022; and all participants completed their second and third data collection by July 2022 and December 2022, respectively. Data were collected from 202 older adults during the first data collection period, with approximate retention rates of 90.1% (n=182) during the second data collection period and 88.1% (n=178) during the third data collection period. Multilevel models and mixed-effects location scale modeling will be used to evaluate the study aims. Project SMART seeks to predict and model the adoption and maintenance of optimal levels of PA and SB among older adults. In turn, this will inform the future delivery of personalized intervention content under conditions where the content will be most effective to promote sustained behavior change among older adults. DERR1-10.2196/47320.