A macromolecular coupling agent containing hydrophilic and hydrophobic groups is made to react with precipitated silica. Interfacial interactions between OH groups of silica and COOH groups of macromolecule are found to be created through either hydrogen bonds alone or through hydrogen bonds and covalent bonds. Aqueous dispersions of unmodified and modified silica are prepared and the colloidal stability and particle size distribution of the dispersions are observed. The dispersions at neutral pH are incorporated into vulcanized/unvulcanized natural rubber latex. The formation of hydrogen bonds and/or covalent bonds is studied via FTIR spectroscopy and their contribution in encouraging filler-rubber interactions is emphasized through mechanical and swelling properties. Uniform distribution and dispersion of modified filler particles throughout the rubber matrix is confirmed by the microstructures of the latex films cast from filler added natural rubber latex. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 40380.