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RESEARCH ARTICLE

A Study on Dual-Response Composite Hydrogels Based

on Oriented Nanocellulose

Lina Dong 1,2† , Mujiao Liang 1,2† , Zhongwei Guo , Anyang Wang , Gangpei Cai , Tianying Yuan ,
2
1,2
1
2
Shengli Mi *, Wei Sun 1,2,3,4 *
2
1 Macromolecular Platforms for Translational Medicine and Bio-Manufacturing Laboratory, Tsinghua-Berkeley Shenzhen
Institute, Shenzhen 518055, P.R. China
2 Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China
3 Department of Mechanical Engineering, Biomanufacturing Center, Tsinghua University, Beijing, P.R. China
4 Department of Mechanical Engineering, Drexel University, Philadelphia, PA, USA
† These authors contributed equally to this work

Abstract: In nature, many biological tissues are composed of oriented structures, which endow tissues with special properties
and functions. Although traditional hydrogels can achieve a high level of biomimetic composition, the orderly arrangement of
internal structures remains a challenge. Therefore, it is of great significance to synthesize hydrogels with oriented structures
easily and quickly. In this study, we first proposed and demonstrated a fabrication process for producing a well-ordered and
dual-responsive cellulose nanofibers + hyaluronic acid methacrylate (CN+HAMA) hydrogels through an extrusion-based
three-dimensional (3D) printing process. CN in the CN+HAMA hydrogels are directionally aligned after extrusion due to
shear stress. In addition, the synthesized hydrogels exhibited responsive behaviors to both temperature and ultraviolet light.
Since the temperature-responsiveness is reversible, the hydrogels can transit between the gelation and solution states while
retaining their original qualities. Furthermore, the developed well-oriented CN+HAMA hydrogels induced directional cell
growth, paving the way for potential applications in ordered biological soft-tissue repair.
Keywords: Nanocellulose hydrogel; Directional arrangement; Thermal response; Ultraviolet response; 3D printing

*Correspondence to: Shengli Mi, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China;
mi.shengli@sz.tsinghua.edu.cn; Wei Sun, Macromolecular Platforms for Translational Medicine and Bio-Manufacturing Laboratory, Tsinghua-
Berkeley Shenzhen Institute, Shenzhen 518055, P.R. China: weisun@mail.tsinghua.edu.cn
Received: March 26, 2022; Accepted: April 21, 2022; Published Online: June 8, 2022
(This article belongs to the Special Issue: Composite/Multi-component Biomaterial Inks and Bioinks)

Citation: Dong L, Liang M, Guo Z, et al. A Study on Dual-Response Composite Hydrogels Based on Oriented Nanocellulose. Int J Bioprint,
8(3):578. http://doi.org/10.18063/ijb.v8i3.578

1. Introduction materials for defect repair of soft tissues with ordered
structures to achieve functional reconstruction .
[2]
Soft-tissue defects are often accompanied by deep Hydrogels, a kind of biomaterial with a three-
tissue injuries, such as muscle, tendon, blood vessel, and dimensional (3D) crosslinking network structure
nerve damage. This requires tissue repair and functional composed of hydrophilic polymers, have been widely used
reconstruction and could lead to local inflammation if not to synthesize biomimetic structures in tissue engineering
handled properly . Soft tissues in living organisms, such as and regenerative medicine [3-5] . Cellulose is widely used
[1]
muscles, nerve tissue, corneal tissue, tendons, and ligaments, in tissue engineering due to its good biocompatibility [6,7] .
have well-ordered microstructures with highly anisotropic Cellulose nanofibers (CNs) are the most commonly used
properties. Defect repair and functional reconstruction of cellulose derivatives in the fabrication of composite
soft tissues with ordered structures is a problem that needs hydrogels. Besides, CNs have been largely used for
to be addressed. Therefore, it is crucial to find biocompatible reinforcing filler to increase the mechanical properties of
© 2022 Author(s). This is an Open-Access article distributed under the terms of the Creative Commons Attribution License, permitting distribution and
reproduction in any medium, provided the original work is properly cited.
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