Several key parameters that influence both the self-healing properties and water retention capacity of biohydrogel networks made of alginate–dopamine (Alg–DA) conjugates have been studied. A judicious combination of biopolymer concentration, dopamine content, pH-dependent cross-linking of catechol groups and the Fe³⁺-coordination of the networks allowed control over the self-healing ability of these bioinspired materials. Moreover, the thixotropic nature of model hydrogels was confirmed using oscillatory rheological loop tests.