Hydrogels are interesting materials for application in biomedicine due to their outstanding properties (e.g., water retention, drug release, and biocompatibility). This work evaluates two series of phosphorus-based hydrogels as potential wounddressing candidates. The materials were synthesized via free-radical polymerization of bis[2-(methacryloyloxy)ethyl] phosphate (BMEP, >= 75 wt %) with (3-acryl amidopropyl)-trimethylammonium chloride solution (APTAC) or 2-acrylamido-2-methyl-1-propane sulfonic acid (AMPS). Due to optimized synthetic conditions, the materials displayed an unprecedented compressive elastic modulus (E') reaching up to 0.19 MPa, which represents a 1000-fold increase compared to previously reported materials. Furthermore, the hydrogels displayed good hydrolytic and enzymatic stability, cytocompatibility using bovine fibroblasts (BFs), and drug loading/release in woundlike pH conditions. In summary, this work demonstrates the potential of phosphorusbased hydrogels as drug-eluting wound-dressing materials.