PVA cryogels are well established as candidate biomaterials for wound healing applications but are not themselves biodegradable or antimicrobial. Blending PVA with NaCMC (CMC) or gelatin (G) can increase the gel’s ability to swell and would introduce a degree of biodegradability. The incorporation of appropriate amounts of a natural antimicrobial/healing agents, such as honey (H), would contribute to the gels properties. The present work addresses the development and characterization of layered gels (PVA-H, PVA-CMC-H and PVA-G-H, with empty PVA, PVA-CMC, PVA-G gels presented as controls). The gels were characterized by FTIR, DSC, in vitro analysis of swelling and microbiological (S. aureus) effects. Addition of gelatin, NaCMC and honey to PVA diminished the PVA chains’ ability to pack into crystallites. Samples containing honey swelled less and presented higher weight loss/biodegradability than samples without honey. Only the honey-laden PVA-CMC and PVA-G presented activity against S. aureus.