The research of starch retrogradation have been attracting interest. Thereby, the long-term retrogradation mechanism (0-21 days) of Pouteria campechiana seed starch (PCSS) was investigated. The results showed that crystal type was changed from A- to B +V-type during retrogradation. The retrogradation PCSS (RPCSS) exhibited faster retrogradation rate and more compact internal ultra-structure compared to rice, wheat and maize starch. Pearson correlation indicated that, as retrogradation days increased, values of & alpha;-1,4-glycosidic bond, A chains, double helix, V-type polymorphism, Mw, relative crystallinity (Rc) and short-range order gradually significantly increased, and B1 chains, B3 + chains values gradually significantly dropped (p < 0.05). These inferred an increasing peak temperature and compactness of morphology with increasing retrogradation days. Compared to native starch, RPCSS & alpha;-1.4-glycosidic bond was increased, which indicated that its quick molecules degradation including decreased Mw, B3 + chains, Rc, semicrystalline order, and & UDelta;H. These might provide a theoretical direction for preparation of starch-basis food.