Hybrid materials are being developed to add organic functionalities to inorganic materials. Here, titanium dioxide is modified with organophosphonic acids (PAs). In several applications, the surface properties of the material play a key role in their performance (e.g. separation, sorption, catalysis). Hence, the surface properties of these materials need to be specifically adjusted to meet the requirements of each application (e.g. in membrane separation or chromatography). As the synthesis conditions have an important influence on the obtained surface properties, it is necessary to understand the impact and differences introduced by altering synthesis conditions. Different solvents are being applied for modification, but a comparative study of the impact of this change in environments is missing in literature. Therefore, our aim is to study the impact of concentration, temperature and pH in water and toluene on the properties of TiO2 modified with propylphosphonic acid (3PA). By combining complementary techniques (DRIFT, TGA and P-31/CP MAS NMR), clear differences induced by the solvent can be found. Moreover, in toluene a lower concentration of 3PA is required to obtain closed packed monolayers than in water. Furthermore, both solvent and concentration are influencing the modification degree and binding type formed on the surface. Moreover, only in water, next to the concentration, also the temperature and pH have a strong impact on the binding type of 3PA. A clear difference in thermal stability of 70 degrees C was found between both binding types. (C) 2016 The Authors. Published by Elsevier B.V.