Asymmetric bilayer membranes have been regarded as ideal wound dressings for skin regeneration. Our previous work reported the potential advantages of polydimethylsiloxane modified gelatin/silicone rubber (PGE/SR) asymmetric bilayer membrane as a wound dressing. However, it is still unknown whether the proportion of the two components of the bilayer membrane has a prominent influence on its relevant performance. Herein, various PGE/SR membranes with different PGE:SR weight ratios (100:25, 100:50 and 100:100) were fabricated through a self‐stratification method driven by surface tension gradients. Subsequently, the effects of the PGE:SR ratios on the relevant performance (i.e. porous structure, mechanical properties, degradability and biocompatibility) of PGE/SR membranes were systematically investigated. The current results demonstrate that the separating force between the PGE and SR components was reduced significantly on increasing the content of SR, and in particular the PGE/SR1 membrane (100:25) exhibited a well‐defined asymmetric bilayer structure with high porosity, appropriate toughness, water uptake, swelling ratio and water permeability. Concomitantly, the maximum weight loss for the PGE/SR1 membrane was ca 70.65% after 9 days of enzymatic degradation, which met the typical healing period of a normal skin wound. In addition, both the original and degraded PGE/SR1 membrane possessed favorable cytocompatibility in vitro, suggesting its potential application as a wound dressing. © 2019 Society of Chemical Industry