The effect of different post-treatments on TiO2 anatase surface reactivity was investigated in order to obtain the best techniques for enhancing anatase performance in diverse applications, e.g., in photocatalysis and especially as photoelectrodes for dye-sensitized solar cells (DSSCs). Different post-treatments of compact anodic anatase TiO2 were compared, including O-2 plasma, UV irradiation, immersion in H2O2, vapor thermal treatment, and post-anodization, evaluating the increase of the amount of OH reactive groups on the surface and removal of surface contamination. In XPS spectra, the increase of OH groups is evident by the O is peak at higher binding energy. ToF-SIMS principal component analysis demonstrated that treatments performed in aqueous media led to a cleaner surface, with substantial removal of electrolyte residues. Stearic acid and the organic dye N719 were adsorbed to the differently post-treated anatase, and adsorption was evaluated by contact angle and dye desorption measurements. A higher loading with molecules containing carboxylic acid functionalities was confirmed by both techniques on the treated samples. The post-treatments that presented the highest amounts of dye were used to prepare photoelectrodes, and these were tested in DSSCs where the efficiency values doubled in comparison with the non-post-treated electrode.