The structured adsorption filter material is one of the ways to enhance the practical applicability of powdered adsorbents, which have limitations in the real water treatment process due to difficulty in the separation process. In this study, three-dimensional (3D) printing technology was applied to prepare filter materials for water treatment processes. A 3D-printed graphene-oxide (GO)-based adsorbent is prepared on a polylactic acid (PLA) scaffold. The surface of the PLA scaffold was modified by subjecting it to strong alkaline or organic solvent treatment to enhance GO doping for realizing effective adsorption of cationic dye solutions. When subjected to 95% acetone treatment, the structural properties of PLA changed, and particularly, two main hydrophilic functional groups (carboxylic acids and hydroxyls) were newly formed on the PLA through cleavage of the ester bond of the aliphatic polyester. Owing to these changes, the roughness of the PLA surface increased, and its tensile strength decreased. Meanwhile, its surface was doped mainly with GO, resulting in approximately 75% methylene blue (MB) adsorption on the 3D-printed GO-based PLA filter. Based on the established optimal pretreatment conditions, a kinetic MB sorption study and an isotherm study were conducted to evaluate the 3D-printed GO-based PLA filter. The pseudo-second-order model yielded the best fit, and the MB adsorption was better fitted to the Langmuir isotherm. These results suggested that chemical adsorption was the main driver of the reaction, and monolayer sorption occurred on the adsorbent surface. The results of this study highlight the importance of PLA surface modification in enhancing GO doping and achieving effective MB adsorption in aqueous solutions. Ultimately, this study highlights the potential of using 3D printing technology to fabricate the components required for implementing water treatment processes.