The relationship between molecular structure and crystalline and lamellar structures of fifteen types of rice starches was studied. GPC and HPAEC were used for the molecular chain analysis and WAXS, SAXS, and CP/MAS ¹³C NMR were employed for aggregation structural analysis. The amylopectin content and the average lengths of fb₁-chains (the degree of polymerization (DP) 13–24) were positively correlated with the amount of double helices (r² = 0.92 and 0.57, respectively). In contrast, amylose content was positively correlated with the amounts of amorphous materials in starch (r² = 0.77). The amount of double helices, which constitute a major part of the crystalline matrix, was positively correlated with the lamellar ordering (r² = 0.81), and negatively correlated with the thickness of crystalline lamellae (r² = 0.90) and lamellar repeat distance (r² = 0.84). Conversely, the amount of the amorphous matrix was correlated with these parameters in the opposite way (r² = 0.50, 0.75, and 0.75, respectively).