Here, the biosorption process for the removal of methylene blue (MB) was developed using three-dimensional printed biocomposite scaffolds obtained from Polylactide / Poly(butylene adipate-coterephthalate) (PLA/PBAT)-immobilized biomass of Chlorella pyrenoidosa (PIBCP). The adsorption capacity of the 3D printed PIBCP was carried out. And the effects of adsorbent dose, initial dye concentration, solution pH, ionic strength, temperature, and contact time on the adsorption performances were discussed. The results show that the decolorization rate for methylene blue on the 3D printed PIBCP30 (with 30% mass of Chlorella pyrenoidosa) is 92.66% at the adsorption time of 24 h. The material also shows a good recyclability to have 72% of removal efficiency after six cycles. Kinetic and adsorption isotherm models indicate that the adsorption of methylene blue onto the 3D printed PIBCP30 occurs mainly through chemisorption. Langmuir maximum adsorption capability of methylene blue on the 3D printed PIBCP30 is calculated to be of 35.21 mg/g (100 mg/g, 298.15 K) . The adsorption is determined to be endothermic and spontaneous. The results indicate that Polylactide/Poly (butylene adipate-coterephthalate) (PLA/PBAT)-immobilized biomass of Chlorella pyrenoidosa (PIBCP) is a promising material for dye removal and the 3D printing technique can be employed to fabricate adsorbent for large-scale wastewater treatment.