Persistence of postoperative adhesions can lead to fatal complications in patients undergoing abdominal and pelvic surgery, even years after the operation. Thus, effective barrier materials are majorly required for reducing peritoneal adhesions. In the present study, a novel bilayer hydrogel achieving both wound dressing and antiadhesion capabilities was developed from gelatin and polyvinyl alcohol (PVA) using simultaneous reagent‐free radiation‐induced crosslinking with γ‐rays. The gelatin presents wound dressing ability, whereas the PVA reveals nonadhesive capability. Layers were sufficiently bonded via a small “mixed” interface, as supported via scanning electron microscopy and 2D‐infrared spectroscopy. Cell culture of 3T3‐Swiss fibroblasts exhibited good cell proliferation on the gelatin, which can further facilitate tissue regeneration, whereas PVA exhibited limited cell adhesion and growth. Cell viability suggests that the bilayer is noncytotoxic. Enzymatic degradation test indicated a complete breakdown of gelatin by proteases, leaving the PVA layer mostly intact. These in vitro assessments of the developed bilayer hydrogel demonstrated its potential as a novel medical material with wound dressing and nonadhesive duality.