In the present paper, the effect of three different types of nano-montmorillonite dispersions (nMt) on the (i) microstructure as witnessed by Scanning Electron Microscopy, (ii) long term density measurements and (iii) pore structure as determined via Mercury Intrusion Porosimetry of Portland – limestone cement formulations have been compared, in an effort to determine the upper and lower bound of nMt addition in cementitious nanocomposites. The reference formulation, contained 60% PC and 40% LS by mass of binder aiming at the minimization of clinker and maximization of other constituents. Two aqueous organomodified NMt dispersions (one dispersed with non-ionic fatty alcohol and the other with anionic alkyl aryl sulphonate) and one aqueous inorganic NMt dispersion (dispersed with sodium tripolyphosphate) were added at 0.5, 1, 2, 4 and 5.5% by mass of solids as replacement of Portland cement. The water to solids ratio was kept constant at 0.3. The inorganic nMt showed the greatest potentials for microstructural enhancement. The way in which the level of the nMt platelet separation affected the pastes was discussed. The research reported was part of a much broader project supported by the EU.