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Understanding the fostering factors of physical activity (PA) and sedentary behavior (SB) in post-stroke chronic survivors is critical to address preventive and health interventions. This cross-sectional study aimed to analyze the association of barriers to PA, fear of falling and severity of fatigue encountered by stroke chronic survivors with device-measured PA and SB. Ambulatory community-dwelling post-stroke subjects (≥six months from stroke onset) were evaluated and answered the Barriers to Physical Activity after Stroke Scale (BAPAS), Short Falls Efficacy Scale-International (Short FES-I) and Fatigue Severity Scale (FSS). SB and PA were measured with an Actigraph GT3X+ accelerometer for ≥seven consecutive days. Stepwise multiple linear regression analysis was employed to identify factors associated with PA and SB. Fifty-seven participants (58.2 ± 11.1 years, 37 men) met the accelerometer wear–time criteria (three days, ≥eight h/day). The physical BAPAS score explained 28.7% of the variance of the prolonged sedentary time (β = 0.547; p < 0.001). Additionally, the walking speed (β = 0.452) together with physical BAPAS (β = −0.319) explained 37.9% of the moderate-to-vigorous PA time (p < 0.001). In chronic post-stroke survivors, not only the walking speed but, also, the perceived physical barriers to PA are accounted for the SB and PA. Interventions to reverse SB and to involve subjects post-stroke in higher levels of PA should consider these factors.