Mortar from the Roman Colosseum and a Roman cistern from Albano Laziale were characterized with optical microscopy, scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FT-IR), and thermal analysis (differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA)). The different techniques provided consistent results that the mortar of the Colosseum is mainly calcareous lime, while the mortar of the cistern is pozzolanic siliceous material. The study highlights the capabilities of the different methods for the analysis of cement. For routine analysis XRD is adequate but for characterization of poorly crystalline phases FT-IR and TGA have definite advantages.