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Here we report the first study of a polypeptide-DNA hybrid supramolecular hydrogel that exhibits these combined favourable properties from both polypeptide-and DNA-components.These hydrogels can be rapidly formed in situ by the simple mixing of two building blocks(i.e.polypeptide-DNA conjugate and complimentary DNA linker)under physiological conditions.Due to the polypeptide-DNA hybrid structures,the resultant hydrogels exhibit multiple-responsiveness to a range of specific physical and biochemical stimuli including temperature,pH,salt,proteases and DNA restriction enzymes.The mechanical strength of the hydrogel can be fine-tuned from several hundred to several thousand Pascal upon rational design,either by tailoring the length of “sticky ends” of DNA linker or by changing the environmental pH,while keeping the total crosslinking density constant.The rapid and gentle in situ formation of the hydrogel by the two components is well-suited for 3D bioprinting to produce designable tissue-like structures containing viable and functional living cells.Biocompatibility of the hydrogels was verified using 3D cell viability assays,signifying its potential application in organ printing.