The development of innovative materials for bone tissue engineering to promote bone regeneration while avoiding fibrous tissue infiltration is of paramount importance. Here, we combined the known osteopromotive properties of bioactive glasses (BaGs) with the biodegradability, biocompatibility, and ease to shape/handle of poly-l-co-d,l-lactic acid (PLDLA) into a single biphasic material. The aim of this work was to unravel the role of the surface chemistry and topography of BaG surfaces on the stability of a PLDLA honeycomb membrane, in dry and wet conditions. The PLDLA honeycomb membrane was deposited using the breath figure method (BFM) on the surface of untreated BaG discs (S53P4 and 13-93B20), silanized with 3-aminopropyltriethoxysilane (APTES) or conditioned (immersed for 24 h in TRIS buffer solution). The PLDLA membranes deposited onto the BaG discs, regardless of their composition or surface treatments, exhibited a honeycomb-like structure with pore diameter ranging from 1 to 5 μm. The presence of positively charged amine groups (APTES grafting) or the precipitation of a CaP layer (conditioned) significantly improved the membrane resistance to shear as well as its stability upon immersion in the TRIS buffer solution. The obtained results demonstrated that the careful control of the substrate surface chemistry enabled the deposition of a stable honeycomb membrane at their surface. This constitutes a first step toward the development of new biphasic materials enabling osteostimulation (BaG) while preventing migration of fibrous tissue inside the bone defect (honeycomb polymer membrane).