Permeability characteristics of the anti-hypertensive drug, diltiazem hydrochloride, from uncross-linked and cross-linked methylcellulose (MC)/graphene oxide (GO) rate controlling membranes (RCMs) were investigated. The MC/GO membranes were cross-linked with different concentrations of glutaraldehyde (GLA) to examine the effect of cross-linking on the permeability characteristics. The ATR-FTIR spectra, along with solubility resistance, swelling studies, the molar mass between cross-links, and moisture absorption of cross-linked RCMs over the uncross-linked RCM confirmed the cross-linking between MC and GO. The cross sectional view of cross-linked and uncross-linked RCMs, as observed by SEM, showed that the porous and fibrillose structure of the uncross-linked RCM was disrupted after cross-linking. The cross-linked RCMs showed improved mechanical and thermal properties compared to the uncross-linked RCMs. In vitro and ex vivo drug release was found to depend on the concentration of the cross-linker, which suggests that drug delivery is controlled by the cross-link density of RCM. © The Royal Society of Chemistry 2016.