The aggregation structure of dye molecules has a great influence on the properties of dye solutions, especially in high concentration. Here, the dye molecular aggregation structures were investigated systemically in aqueous solutions with high concentration using three reactive dyes (O-13, R-24:1 and R-218). O-13 showed stronger aggregation than R-24:1 and R-218. This is because of the small non-conjugate side chain and its β-linked position on the naphthalene of O-13. Compared with R-218, R-24:1 showed relatively weaker aggregation due to the good solution of R-24:1. The change of different aggregate distributions in the solutions were also investigated by splitting the absorption curves. Moreover, it is found that the surface tension of solutions can be modified by the combined effect of both aggregation and the position of the hydrophilic group, which, however, also have an effect on viscosity. This exploration will provide guidance for the study of high concentration solutions.