Understanding the interlayer interaction between 2D layered structures is critical for the construction of various micro- and nanoscale functional devices. However, both the normal and the tangential interlayer interactions between 2D layered materials have rarely been studied simultaneously. In this work, an immersion and lift-up method is proposed to wrap a layer of graphene flakes onto a plasma-pretreated atomic force microscopy (AFM) nanoprobe for the measurements of interaction forces by AFM. The normal interactions (adhesion force and adhesion energy) and tangential interactions (friction force) between two different probes (Pt-coated probe and graphene-wrapped probe) and two different 2D graphene materials [graphene and graphene oxide (GO)] were systematically measured, respectively. The adhesion energies of Pt–GO, Pt–graphene, graphene–GO, and graphene–graphene were measured to be 0.72 ± 0.05, 0.41 ± 0.03, 0.19 ± 0.02, and 0.10 ± 0.02 J m–2, respectively. The graphene–graphene contact pair showed the lowest adhesion force (5.57 ± 1.03 nN) and adhesion energy (0.10 ± 0.02 J m–2), which was attributed to the strong covalent bonds and charge density distribution. The friction coefficients of Pt–GO, graphene–GO, Pt–graphene, and graphene–graphene were determined to be 0.38, 0.14, 0.054, and 0.013. The graphene–graphene tribo-pair exhibited a superlow friction state for a long time, which was attributed to incommensurate contact and weak van der Waals interactions. These findings provide a technical route to reveal the interlayer interactions of various 2D layered materials, which can be widely applied in microelectromechanical systems.