Zeolite-A was synthesized successfully from kaolinite and hybridized with two species of biopolymers (chitosan (CH/Z) and β-cyclodextrin (CD/Z)). The obtained hybridized forms were assessed as potential adsorbents of Congo red synthetic dye (CR) with enhanced affinities and elimination capacities. The synthesized CD/Z and CH/Z hybrids demonstrated uptake capacities of 223.6 and 208.7 mg/g, which are significantly higher than single-phase zeolite-A (140.3 mg/g). The integrated polymers change the surface area, surface reactivity, and number of free active receptors that are already present. The classic isotherm investigations validate Langmuir equilibrium behavior for ZA and Freundlich properties for CD/Z and CH/Z. The steric parameters validate a strong increase in the existing active receptors after the incorporation of CD (CD/Z) to be 98.1 mg/g as compared to 83 mg/g for CH/Z and 60.6 mg/g for ZA, which illustrate the detected uptake behaviors. Moreover, the CR dye was adsorbed as several molecules per single site, reflecting the vertical uptake of these molecules by multimolecular mechanisms. The energetic assessment, considering both Gaussian energies and adsorption energies (<40 kJ/mol), validates the dominant impact of the physical mechanism during the sequestration of CR (dipole binding interactions (2-29 kJ/mol) and hydrogen bonds (<30 kJ/mol)), in addition to the considerable effect of ion exchange processes. Based on the thermodynamic parameters, the CR molecules were adsorbed by exothermic and spontaneous reactions.