Palygorskite (PAL) as a natural one-dimensional nanomaterial has attracted tremendous attention as reinforcement agent in polymer nanocomposites. But its intrinsic existing form of aggregates or bundles and hydrophilic properties, highly requires an eco-efficient and environmentally benign approach for both of the disaggregation and organo-modification of PAL. We report a facile and effective process to achieve individualized organo-modified PAL fibers. It was carried out through surface modification reactions in the form of PAL iso-propanol gels with various alkyl and functional silanes. In contrast to the modifications in highly toxic solvent of toluene, reactions in iso-propanol make it possible to modify the surface of individual PAL fibers to obtain isolated organo-modified PAL fibers. With such a relatively green procedure, even higher amount of organic substituent has been grafted on to the surface of PAL fibers. Consequently, excellent dispersion of modified PAL nanofibers in acrylate polymer coatings was achieved, which exhibits outstanding corrosion protection properties.