Natural polymers are reliable compounds in drug delivery systems (DDS). Herein, two series of safe and reliable polyelectrolyte hydrogels (PEHs) were prepared from two oppositely charged polysaccharides, namely tragacanth (TG) and chitosan (CS), and applied for the delivery of ibuprofen as a model drug. Considering the different interactions of CS and TG as a polycation and a polyanion, respectively, with the drug, herein, two series of PEHs were prepared, and their diversity in morphology and drug release ability were studied. The system provided a high percentage of drug loading efficiency (>90%) and was sensitive to the acidity of different media. The drug release pattern was favorable; the data showed that the slowest rate of drug release was obtained at pH = 1.2, followed by pH = 5.4, and fastest drug release occurred at a slightly basic pH (=7.4); the mechanism of drug release was studied using different kinetic models, where at pH = 1.2 and 7.4, the drug release curve best matched the zero order and the Hixson–Crowell model, and at pH = 5.4, the Weibull model represented the perfect agreement with the drug release patterns. The stability of the drug carrier was explored by fluorescence imaging. The cytotoxicity of the CS-I-T 30% and CS-T composites was evaluated towards the cultured MCF7 cells for 24 and 48 h, and no toxic effects were observed.