Hydrogen/deuterium isotopic substitution neutron diffraction techniques have been used to measure the solute-solute intermolecular structural correlations in 0.06, 0.11, and 0.16 mole fraction tertiary butanol-water solutions. Empirical potential structure refinement (EPSR) procedures have been used to extract detailed information relating to the intermolecular structure in these systems. A trend from hydrophobic to hydrophilic character of the solute-solute correlations as a function of solute concentration is observed. Of particular note is the domination of nonpolar to nonpolar solute contacts at 0.06 mole fraction concentration compared with a more complex mixture of nonpolar and polar solute-solute intermolecular contact configurations at the higher alcohol concentration.