Hydrogels are the most appealing candidates of biomaterials for bioprinting. In this field of bioprinting, the lack of suitable hydrogels remains a major challenge. Thus, choosing appropriate hydrogels is the key to successfully print self-supporting 3D constructs. Most importantly, the design criteria regarding the bioinks and the obtained constructs should be made clear in advance. Therefore, the first task of this study is to clarify the design criteria regarding the important properties of a potential bioink and the generated 3D construct, including rheological, interfacial, structural, biological, and degradation properties, which are crucial for printing of complex and functional 3D structures. A method is developed for evaluating the printability of a candidate hydrogel through simulating its rheological behaviors before, during, and after printing. After that, two novel strategies are proposed in order to obtain multilayered hydrogel constructs with strong interface bonding. In the first strategy, trisodium citrate (TSC) acts as a chelating agent to remove the superficial Ca 2+ at each layer. The subsequent post-crosslinking of constructs in a calcium chloride bath will further create the crosslinks and enhance the adhesion between adjacent layers. The second strategy for improving the adhesion between printed layers of a construct is to exploit the interaction between two oppositely charged hydrogels. On the basis of these two strategies, the exciting results have been obtained, which include strong interfacial bonding between two layers of the printed structures, good shape fidelity Even though I have put in great effort for completion of this thesis, it would not have been possible without the support and help of many individuals and organizations. I would like to extend my sincerest thanks to all of them. Firstly, I would like to express my gratitude to my supervisor, Prof. Lin Li for giving me an opportunity to be his student. His valuable guidance, warm encouragements motivated me to conduct experiments, write papers and complete my thesis. I have benefitted much from his rigorous attitude towards scientific research. Special thanks are given to my lab mate and close friend, Dr. Yu Jun Tan, for her assistance, knowledge sharing and valuable discussion. I also appreciate my group member Dr. Sijun Liu, who provides his assistance during my PhD study. My appreciation also goes to the other two group members, Mr Anil Kumar Bastola and Miss Ying Zhen Low, for their encouragement and accompany.