A series of porous materials made of sodium alginate have been synthesized by freeze‐drying including rhodamine B as pigment complexed or not with the aromatic polymer poly(sodium 4‐styrenesulfonate). By means of aromatic‐aromatic interactions between the aromatic polymer and the dye, the luminescent properties of the final materials can be controlled. This is mainly produced by avoiding the dye self‐aggregation in the solid state in a higher extent as the excess of the aromatic polyelectrolyte over the dye increases. The solid materials present a structure made of microsheets and microfibers of alginate, density ranging between 17 and 26 mg/cm3, porosity higher than 97%, and Young's modulus ranging between 8 and 24 kPa. This work highlights the role or aromatic polyelectrolytes to control properties of both the polymer and its aromatic counterions in the solid state, making use of aromatic‐aromatic interactions.
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