Guided bone regeneration (GBR) membranes favor periodontal regrowth, but they still have certain limitations, such as improper biodegradation and poor mechanical property. To overcome these shortcomings, we have generated a unique multifunctional membrane. A polycaprolactone/gelatin/β-TCP and alginate/gelatin trilayered construction was fabricated through electrospinning and casting technology. The prepared membranes have suitable physicomechanical and in-vitro properties to confirm the compatibility of the product in the body. Phase analysis, functional groups, surface microstructure, and contact angle were measured as basic characteristics. For a mechanical performance evaluation, the tensile strength at suturing point was measured through pullout tensile strength test, and it showed the suture capability of bi-layered membranes. Highest tensile strength for A75G25 was recorded with 2.9 ± 0.15 MPa with 105% strain. Further, the osteoblast and fibroblast-type cell toxicity results showed that the electrospun membrane offered compatible environment to cells while the alginate sheet was found to be sufficiently capable to suppress the cellular attachment while also being a nontoxic material. Post-implantation, according to the in-vivo conclusions of the tri-layered membrane, there was appreciable bone formation. Compared to an implant without membrane covering, enhanced new bone formation can be identified after 8 weeks of implantation with P1G4β10 membranes-covered site.