Geopolymers are a class of aluminosilicate materials synthesized by alkaline or alkali-silicate activation of solid alumina-and silica-containing precursor materials at ambient or higher temperature. These products have highly significant commercial and technological potential, but the exact physicochemical nature of the geopolymeric binder phase has never before been determined. Through analysis of existing experimental results from the literature and comparison with related systems, in particular the hydrothermal synthesis of zeolites, geopolymeric binders are identified as being comprised of agglomerates of nanocrystalline zeolites compacted by an amorphous gel phase. The degree of crystallinity is largely determined by product formulation and synthesis conditions. Results from powder X-ray diffraction, microscopy, electron diffraction, mechanical strength testing, and calorimetry are analyzed and shown to be consistent with the theory presented. The implications of nanocrystallinity are discussed, and areas to be targeted in further experimental investigations are identified.