An in situ characterization method for mechanical and adhesive properties of organic/ceramic composite membranes is built on the basis of nanoindentation technique in this work. The polydimethylsiloxane (PDMS) was used as the separation layer with the support of porous ZrO2/Al2O3 ceramic tubes. The effects of roughness of the ceramic support and the viscosity of PDMS solution on the mechanical properties of the PDMS separation layer and the interfacial adhesion at the interface were investigated in detail. It was found that when the roughness of the ceramic support increased and the viscosity of PDMS solution decreased, the interfacial adhesion strength of PDMS/ceramic composite membrane increased, but these two variables had little effect on the mechanical properties of the PDMS separation layer. Our results indicate that the mechanical interlocking dominates the adhesion between the PDMS separation layer and the porous ceramic support. (C) 2009 American Institute of Chemical Engineers AIChE J, 56: 1584-1592, 2010