There are many commercially importantmultiphasematerialswhich contain amorphous phases, such as cement pastes, porcelains, glass-ceramics or pharmaceutical compounds. However, the analysis of amorphous phase(s) within cement matrices that contain high amounts of crystalline phase(s) is a challenge. Here, we report measurements of total scattering data quantitatively analyzed by Pair Distribution Function (PDF) minimization and Rietveld methodology to determine phase compositions including both amorphous and nanocrystalline phase contents in cement-related samples. Furthermore, laboratory techniques were used to complement the sample characterization. In addition to five reference materials, the main phase of calcium aluminate cements, CaAl2O4 hydrated at 50 ??C to yield crystalline hydrogarnet, Ca3Al2(OH)12, (43wt%) and nanocrystalline aluminum hydroxide gel, Al(OH)3??0.1H2O (50wt%)was also investigated. The PDF analyses revealed that the hydroxide gel has a gibbsite local structurewith an average particle size close to 5 nm. PDF and Rietveld quantitative phase analysis results fully agree.