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Objective: Using self-determination theory (SDT), we examined relationships between cardiac rehabilitation (CR) participants’ perceived autonomy support, motivation for exercise, and exercise behavior. Research Method/Design: Male CR outpatients (N = 53; Mage = 62.83 ± 10.78 years). The design was correlational (cross-sectional and prospective), examining relationships between perceived autonomy support and motivation for exercise at Week 4 of CR participation as well as motivation and CR attendance and other indicators of exercise behavior (frequency, duration, total exercise time) at a 1-week follow-up, 10 weeks later. Results: Perceived autonomy support was correlated with self-determined motivation, r(53) = .32, p < .05. Self-determined motivation predicted total exercise volume at follow-up, r(53) = .34, p < .05, as well as length of exercise session duration (R2 = .27; β = .52, p < .001). Conclusion: Results support SDT and the potential for autonomy support from interventionists to affect self-determined motivation and exercise behavior of participants involved in CR.