A synthesized MIL-101-NH2 has been used as an adsorbent to analyze Congo red (CR), methyl orange (MO), and acid chrome blue K (AC) dye adsorption phenomena. This investigation, based on statistical physics treatment, applied the double layer model with two energies to understand dye adsorption on three samples, namely, MIL-101-NH2-1, MIL-101-NH2-2, and MIL-101-NH2-3, at T = 298 K. Modeling results indicated that dye adsorption occurred via a mixed adsorption orientation for CR and MO dyes and a non-parallel orientation for AC dye on the MIL-101-NH2 surface. Dye uptake quantities varied from 2534.4 to 3440 mg/g for CR dye, 240.4 to 490.8 mg/g for MO dye, and 277 to 293 mg/g for AC dye. Thus, the highest adsorption amount appeared in the case of CR dye. Interpretation of the calculated energies showed that adsorption of the dyes on MIL-101-NH2 is a physisorption phenomenon, which could be controlled through energetic parameters obtained via numerical findings using the statistical double layer model. Moreover, the expression of the model is exploited to investigate the thermodynamic functions, such as internal energy.