As an eco-friendly material, Zn-adeninate bio-metal-organic framework (bio-MOF) was investigated as an efficient adsorbent for both anionic and cationic dyes. The adsorption capability of the synthesized Zn-adeninate bio-MOF was confirmed by its notable surface area of 52.62 m2 g−1 and total pore volume of 0.183 cm3 g−1. The bio-MOF adsorption profiles of anionic direct red 81 (DR-81) and cationic methylene blue (MB) dyes were investigated under different operating parameters. The optimum dosages of Zn-adeninate bio-MOF were 0.5 g L−1 and 1 g L−1 for MB and DR-81 decolorization, respectively. The pHPZC of Zn-adeninate bio-MOF was 7.2, and maximum monolayer adsorption capacity was 132.15 mg g–1 for MB, which decreased to 82.54 mg g–1 for DR-81 dye. Thermodynamic data indicated the spontaneous and endothermic nature of the decolorization processes. Additionally, the adsorption processes were in agreement with the Langmuir and pseudo-second-order kinetic models. The synthesized Zn-adeninate bio-MOF could be reused several times with high decolorization ability. These findings demonstrated that the synthesized Zn bio-MOF is an effective and promising adsorbent material for the removal of both cationic and anionic dyes from polluted water.