The term “macro-defect-free” refers to the absence of relatively large voids (or defects) that are normally present in conventional cement pastes due to entrapped air or inadequate mixing. A decade ago, Birchall and co-workers developed a novel processing method that avoids the formation of these strength-limiting defects. This method, outlined schematically in Figure 1, consists of mixing hydraulic cement powder, a water-soluble polymer, and a minimal amount of water under high shear to produce a macro-defect-free (MDF) cement composite. Several cement/polymer systems can be processed by this flexible technique, although the calcium aluminate cement/polyvinyl alcohol-acetate (PVA) copolymer system is most common: MDF cements display unique properties relative to conventional cement pastes. For example, the flexural strength of MDF cement is more than 200 MPa as compared to values on the order of 10 MPa for conventional pastes. One can view MDF cements as a type of “inorganic plastic.” As is the case with plastic processing, fillers such as alumina, silicon carbide, or metal powders can be added to MDF cement to modify its performance properties (e.g., abrasion resistance, thermal or electrical conductivity, and hardness). The combined attractiveness of inexpensive raw materials and flexible, low-temperature processing has generated great interest in this new class of advanced cement-based materials.