Mechanical and degradation properties are crucial factors of guided tissue/bone regeneration (GTR/GBR) membranes. In this work, a series of fibrous membranes with different ratios of polycaprolactone (PCL) and gelatin (Gel) were prepared (PCL:Gel = 1:9 (P1G9), 3:7 (P3G7), 5:5 (P5G5), 7:3 (P7G3), and 9:1 (P9G1)) by electrospinning, and their physicochemical properties and in vitro degradation behaviors were systematically investigated. Mechanical tests showed that tensile strength was enhanced with the presence of Gel, and the tensile strength of the P9G1 membrane reached nearly three times that of the pure PCL membrane. The degradation rate of the composite membranes could be adjusted by controlling the ratio of PCL and Gel; the higher the Gel content was, the faster the degradation of the PCL/Gel membrane. The higher PCL content favored maintaining the fibrous structure of the electrospun membranes. These findings will be beneficial for designing PCL/Gel composite materials for biomedical applications.