Molecular dynamics simulations are used to investigate the physisorption of organic friction modifiers (OFMs) lubricated by 1-decene trimer (PAO4) representing a base oil and confined between hydroxylated SiO2 (001) surfaces. The results indicate that OFM molecules form dense, tendentiously vertical monolayer films at low temperature but loose adsorption layers at high temperature, particularly for R-NH2 with weaker molecular polarity. The structural information is quantitatively clarified by mass density profiles, radial distribution function, and probability distributions of an end-to-end distance at a perpendicular-to-surface direction. The movement performance of lubricant, reflected by the thickness of the organic part and radius of gyration of PAO4 molecules, strongly depends on temperature. The adsorption amount of OFM molecules decreases dramatically with lowering OFM polarity and increasing temperature above the critical desorption temperatures of about 320, 373, and 453 K for amine (R-NH2), alcohol (R-OH), and acid (R-COOH), respectively. The interaction energies of the OFM-surface decrease continuously for the R-NH2 system with temperature and decrease rapidly as temperature exceeds a critical value for both R-OH and R-COOH systems. The single-molecule geometry optimization validates the significant role of the electrostatic and hydrogen-bond attractions in molecular adsorption. Therefore, the OFMs with stronger polarity (like R-COOH) present stronger adsorption and better temperature resistance. The findings in this work are of particular value and provide a guideline in designing and engineering novel OFM additives for extreme lubrication conditions.