Treating wound infections has been a difficult task ever since pathogenic bacteria started to develop resistance to common antibiotics. The present study develops hybrid hydrogels based on the formation of a polyelectrolyte complex between the anionic charges of dopamine‐functionalized Gellan Gum (GG‐DA) and the cationic moieties of the TMP‐G2‐alanine dendrimer. The hydrogels thus obtained can be doubly crosslinked with CaCl2, obtaining solid hydrogels. Or, by oxidizing dopamine to GG‐DA, possibly causing further interactions such as Shiff Base and Michael addition to take place, hydrogels called injectables can be obtained. The latter have shear‐thinning and self‐healing properties (efficiency up to 100%). Human dermal fibroblasts (HDF), human epidermal keratinocytes (HaCaT), and mouse monocyte cells (RAW 264.7), after incubation with hydrogels, in most cases show cell viability up to 100%. Hydrogels exhibit adhesive behavior on various substrates, including porcine skin. At the same time, the dendrimer served to crosslink the hydrogels and endow them with excellent broad‐spectrum microbial eradication activity within four hours, evaluated using S. aureus 2569 and E. coli 178. Using the same GG‐DA/TMP‐G2‐alanine ratios hybrid hydrogels with tunable properties and potential for wound dressing applications can be produced.This article is protected by copyright. All rights reserved