Nanoscale deformation behavior of aluminum at sliding interface was investigated by nanoscratch experiment and X-ray photoelectron spec-troscopy (XPS) in variable conditions involving dry, water and aqueous H2O2, which has not been discussed previously. It was found that deformation of aluminum in the nanoscratch process could be divided into two regimes relying on the evolution of frictional coefficient. Similar results have been observed in dry and water conditions. However, the stick-slip behavior is integrated into deformation process with aqueous H2O2 compared with the results of that in dry and water conditions, resulting from the formation and breaking of chemical bonds interaction of OH and Al atom. In addition, this deformation behavior is described in the framework of a mathematical model based on Mo's theory using the atomic contact concept instead of asperity contact, which relates the transition of friction from sub-linear to linear and deformation changing from elastic to changing elastic-plastic. Finally, a parameter of critical energy barrier is employed to reveal the atomic material removal mechanism in Al chemical mechanical planarization (CMP) process with the consideration of chemical actions and nanoscale deformation behavior.