3D Printing becomes an attractive toolbox for fabricating highly complex structure useful for soft tissue engineering, biocatalysis, and bioenergy. This research aims to develop versatile and effective bio-inks for printing living microorganisms (cells, yeast, algae) or biomolecules (enzyme, protein, DNA) from both naturally derived materials, such as collagen, alginate, gelatin, cellulose and functionalizable synthetic polymers such as FDA-approved pluronic and zwitterionic polymers. Gelation under mild condition to form 3D-bioprinted hydrogel with satisfactory mechanical property, shape integrity and preserved bioactivity is also explored. The obtained fundamental knowledges would pave a way to 4D printing, enabling the development of smart /stimuli-responsive materials.