Inspired by reversible networks present in nature, we have explored the printability of catechol functionalized polyethylene glycol (PEG) based inks with metal-coordination crosslinking. Material formulations containing Al 3+ , Fe 3+ or V 3+ as crosslinking ions were tested. The printability and shape fidelity were dependent on the ink composition (metal ion type, pH, PEG molecular weight) and printing parameters (extrusion pressure and printing speed). The relaxation time, recovery rate and viscosity of the inks were analyzed in rheology studies and correlated with thermodynamic and ligand exchange kinetic constants of the dynamic bonds and the printing performance (i.e. shape fidelity of the printed structures). The relevance of the relaxation time and ligand exchange kinetics for printability was demonstrated. Cells seeded on the crosslinked materials were viable, indicating the potential of the formulations to be used as inks for cell encapsulation. The proposed dynamic ink design offers significant flexibility for 3D (bio)printing, and enables straightforward adjustment of the printable formulation to meet application-specific needs.Włodarczyk-Biegun et al 2 dynamics by varying the metal ion or the pH of the system [3], leading to networks with adjustable mechanical properties [11]. Metal complexation is widely used in natural materials to tune mechanical strength of bulk and interface materials. [3] One of the most prominent examples is the metal-catechol interaction in the DOPA-reach mussel adhesive proteins. The catechol-metal interaction takes place in seawater due to the mild basic pH and the presence of metal ions, and leads to fast gelation of the secreted proteinaceous fluid. In a similar way, catechol-functionalized polymers mixed with metal ions (V 3+ , Fe 3+ , Al 3+ ) have been demonstrated to show pH-tunable crosslinking degree, fast network formation and self-healing behavior. [12,13] The mechanical properties (e.g. shear modulus, relaxation time) of the formed polymer network can be finely tuned by the type of metal ion and pH. [13,14] Only a few reports have exploited metal-ligand coordination complexes to obtain printable hydrogels [3,11,15]. The bisphosphonate-Ca 2+ interaction has been used to print bisphosphonate-functionalized hyaluronic acid (HA-BP) at pH 7 [11]. The reversible gel composed of 2.7% w/v HA-BP and 200 mM CaCl 2 was printable and scaffolds with four layers, with strand diameter of ca. 1 mm, were obtained without the need of further crosslinking. The gels were stable in PBS solution at pH 7 for 1 day but softened and dissolved within hours at lower pH. This is due to the protonation of bisphosphonate at decreasing pH, and the weakening of bisphosphonate-Ca 2+ coordination. Crosslinking with Ag 2+ was tested as an alternative [16], however the printability was not assessed. In a different work, the carboxyl-Fe 3+ interaction was used to stabilize poly(acrylamide-co-acrylic acid) printed structures by immersing the prints in the metal ion salt, leading to robust gel formation ...