The present invention relates to a thermoplastic cellulose composite for additive manufacturing. The composite comprises at least 50 weight-% of total cellulose, a plasticizer, and a coupling agent of an epoxy-modified polyunsaturated fatty acid. The material is fully bio-based and offers improved cellulose content and thermal resistance compared to existing bio-based thermoplastic materials used in additive manufacturing.

Herein disclosed is a method of printing a 3D freeform structure in an embedding medium. The method includes providing an ink composition in a nozzle, wherein the ink composition includes a thermoplastic, a non-thermoplastic, a thermally degradable polymer, and/or a thermosensitive polymer, dissolved in a solvent; dispensing the ink composition through a nozzle into the embedding medium to precipitate a printed structure from the ink composition, wherein the ink composition exits from the nozzle directly in the embedding medium; and maintaining the printed structure in the embedding medium until the immersion precipitation is completed for forming the 3D freeform structure. A system operable to carry out the method is also disclosed. The system includes a syringe coupled to a nozzle.