Electrospinning of poly(L-lactic acid) (PLLA) and gelatin separately to form nonwoven PLLA or gelatin nanofibrous membranes was investigated. Factors that could affect the fiber morphology and fiber diameter were studies for PLLA and gelatin, respectively. The polymer solution concentration was found to play a dominant role in the formation of defected or nondefected ultrafine fibers. Using a specially designed experimental setup with separate syringe pumps for polymer solutions and separate power supplies for high voltages for electrospinning, PLLA-gelatin bicomponent fibrous membranes were formed with PLLA fibers interweaving with gelatin fibers. Multicomponent fibrous scaffolds can be very useful for tissue engineering and/or controlled release applications.