AbstractExperiments on molecular deposition (MD) films with and without alkyl terminal groups deposited on silicon wafers were conducted using nano‐indentation. It was found that MD films and alkyl‐terminated MD films exhibit a higher critical load and a lower coefficient of friction than the silicon substrate. The critical load increases with the number of layers, and the coefficients of friction of MD films with alkyl terminal groups are lower than those of the corresponding MD films with the same number of layers but without alkyl terminal gro