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Abstract Background The present study assessed physical activity (PA) and sedentary behavior (SB) levels and their motivational and emotional health-related correlates, in outpatients following a cardiovascular rehabilitation (CR) program, and compared these variables with those of a healthy control group. Methods The study included 119 participants: 68 CR outpatients (M age 57.76 ± 10.76; 86.76% males) and 51 control participants matched on age (M age 57.35 ± 6.33 years; 45.10% males). PA and SB were assessed using accelerometers during the first week post-discharge for outpatients and during a typical week for controls. Motivational (i.e., perceived capabilities, affective and instrumental attitudes, intention, approach-avoidance tendencies) and emotional health-related variables (i.e., anxiety, depressive symptoms, fatigue, pain intensity) were measured using validated scales. PA and SB data from 17 outpatients and 42 controls were valid for analysis, resulting in a final sample of 59 participants. Results CR outpatients engaged an average of 60.21 (± 34.79) min of moderate-to-vigorous PA (MVPA), and 548.69 (± 58.64) min of SB per day, with 18 more minutes of MVPA per day than controls (p = .038). Univariate and multivariate regressions indicated that positive affective attitudes were associated with higher MVPA (b = 10.32, R2 = 0.07, p = .029), and that males spent more time in SB than females (b = 40.54, R2 = 0.09, p = .045). Univariate and multivariate logistic regressions showed that meeting the World Health Organization’s weekly guidelines for MVPA was associated with higher perceived capabilities toward PA and more positive affective attitudes (OR = 1.17, p = .030; OR = 1.26, p