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The purposes of this study were to determine the moderation effects of affective attitude on the effects of cognitive attitude and intention on leisure-time moderate-to-vigorous physical activity (MVPA). 2100 undergraduate students participated in this study. The hierarchical regression analyses and moderation analyses showed that affective attitude significantly moderated effects of cognitive attitude on MVPA. It suggested that when affective attitude was negative, the effect of cognitive attitude on MVPA was not significant; when it was positive, the higher the value of affective attitude score, the larger the effects of cognitive attitude on MVPA. The results also showed that affective attitude significantly moderated effect of intention on MVPA and the indirect effects of cognitive attitude on MVPA through intention.