3D Printing of Self‐Assembling Nanofibrous Multidomain Peptide Hydrogels

3D printing has become one of the primary fabrication strategies used in biomedical research. Recent efforts have focused on the 3D printing of hydrogels to create structures that better replicate the mechanical properties of biological tissues. These pose a unique challenge, as soft materials are difficult to pattern in three dimensions with high fidelity. Currently, a small number of biologically derived polymers that form hydrogels are frequently reused for 3D printing applications. Thus, there exists a need for novel hydrogels with desirable biological properties that can be used as 3D printable inks. In this work, the printability of multidomain peptides (MDPs), a class of self‐assembling peptides that form a nanofibrous hydrogel at low concentrations, is established. MDPs with different charge functionalities are optimized as distinct inks and are used to create complex 3D structures, including multi‐MDP prints. Additionally, printed MDP constructs are used to demonstrate charge‐dependent differences in cellular behavior in vitro. This work presents the first time that self‐assembling peptides have been used to print layered structures with overhangs and internal porosity. Overall, MDPs are a promising new class of 3D printable inks that are uniquely peptide‐based and rely solely on supramolecular mechanisms for assembly. Multidomain peptides (MDPs), a class of self‐assembling peptides, are used to 3D print complex, 3D structures. Multiple MDPs are demonstrated as printable, and oppositely charged MDPs are printed together into layered, porous constructs. MDPs are found to support high cell viability regardless of charge, while charge is shown to influence cellular behavior and morphology.