Metal-organic frameworks (MOFs) have advanced several applications, including energy, biomedical and environmental remediation. However, most of the reported MOF materials are in powder form limiting their applications. This study reported the processing of MOF via three-dimensional (3D) printing of cellulose-MOFs (denoted as CelloMOFs). The 3D printing procedure involved a one-pot method including three steps: gel formation, 3D printing, and in-situ growth of MOF crystals. This procedure offered 3D printing of CelloMOF via a binder-free method with high loading of 67.5 wt%. The 3D-printed porous structures were used as adsorbents for carbon dioxide (CO₂), dye, and heavy metal ions. They can be also used as catalysts for the degradation of water pollutants such as organic dyes. The materials can be separated easily without requiring extra procedures such as centrifugation or filtration. The materials offered complete (>99%) removal of organic dyes within 10 min with high selectivity toward anionic dyes e.g, methyl blue (MeB). The materials exhibited CO₂ and heavy metal ions adsorption capacities of 0.63 mmol/g (27.7 mg/g) and 8–328 mg/g, respectively, with good recyclability. Our methodology will open new venues for advanced 3D printing of CelloMOF and its applications for water treatment and air purification.