It is obvious that maltitol, like other disaccharides, owes some of its functional properties to structural features such as the flexibility of the glycosidic bond and hydrogen bonding and to its aqueous solution physicochemical properties, especially solubility and metastable zone width. This is particularly the case for molecular arrangements, which take place before and during crystallization process. We have previously used FTIR spectra to study structural properties of the maltitol molecule in concentrated solution like molecular associations or changes in conformation [1]. To complement these molecular properties, the different maltitol solution physicochemical properties having a relationship with maltitol-water or maltitol-maltitol interactions like solubility, metastable zone width, viscosity, and density were determined [2]. In this work we used these physicochemical results to optimize maltitol crystallization both by reducing the process duration and by improving the obtained crystal quality. Two strategies have been tested: the optimization of the time/temperature profile during the classical cooling crystallization and the application to maltitol of evaporative crystallization, a process usually used for sucrose preparation. The obtained results mainly showed remarkable difference in crystal mean size and crystal size distribution when the cooling profile was modified. On the other hand, evaporative crystallization was shown to make it possible to lower considerably the crystallization time compared to the cooling process but crystal morphological properties seem to be considerably modified by evaporation.