The thermal and hydrolytic degradation of electrospun gelatin membranes cross-linked with glutaraldehyde in vapor phase has been studied. In vitro degradation of gelatin membranes was evaluated in phosphate buffer saline solution at 37 ºC. After 15 days under these conditions, a weight loss of 68 % was observed, attributed to solvation and depolymerization of the main polymeric chains. Thermal degradation kinetics of the gelatin raw material and as-spun electrospun membranes showed that the electrospinning processing conditions do not influence polymer degradation. However, for cross-linked samples a decrease in the activation energy was observed, associated with the effect of glutaraldehyde cross-linking reaction in the inter- and intra-molecular hydrogen bonds of the protein. It is also shown that the electrospinning process does not affect the formation of the helical structure of gelatin chains. ; This work was supported by FEDER through the COMPETE Program and by the Portuguese Foundation for Science and Technology (FCT) in the framework of the Strategic Project PEST-C/FIS/UI607/2011 and by projects project references NANO/NMed-SD/0156/2007 and PTDC/CTM-NAN/112574/2009. The authors also thank support from the COST Action MP1003, 2010 ‘European Scientific Network for Artificial Muscles’. DMC, JP and VS would like to acknowledge the FCT for the SFRH/BD/ 82411/2011, SFRH/BD/64901/2009 and SFRH/BD/64901/2009 grants respectively.