Abstract: Interface adhesion toughness between multilayer graphene films and substrates is a major concern for their integration into functional devices. Results from the circular blister test, however, display seemingly anomalous behaviour as adhesion toughness depends on number of graphene layers. Here we show that interlayer shearing and sliding near the blister crack tip, caused by the transition from membrane stretching to combined bending, stretching and through-thickness shearing, decreases fracture mode mixity G
I, leading to lower adhesion toughness. For silicon oxide substrate and pressure loading, mode mixity decreases from 232% for monolayer films to 130% for multilayer films, causing the adhesion toughness G
c to decrease from 0.424 J m−2 to 0.365 J m−2. The mode I and II adhesion toughnesses are found to be G
Ic = 0.230 J m−2 and G
IIc = 0.666 J m−2, respectively. With point loading, mode mixity decreases from 741% for monolayer films to 262% for multilayer films, while the adhesion toughness G
c decreases from 0.543 J m−2 to 0.438 J m−2. The reason why the surface adhesion of a graphene monolayer is much greater than that of graphene multilayers remains unclear. Here, the authors build a model to show interlayer sliding and fracture mode mixity cause the decrease in adhesion toughness of multilayer graphene.