The use of nanotechnology ( and nanocomposites and nanohybrids) in replacing cement with nanomaterials due to environmental aspects and reduction of pollutants is presently an important issue and of course a significant problem in the whole world. In this regard, the effect of various weight percentages of functionalized carbon nanotubes together with montmorillonite nanoparticles and with titanium oxide nanoparticles were studied as replacements for the cement to improve the mechanical and microstructural properties of hardened cement paste composites. In the present study, carbon nanotubes, TiO2, and montmorillonite nanoparticles were synthesized as additions into cement matrix, and their nano-structural characterizations were studied using the TEM, XRD, X-Powder, DSC-TGA, FTIR, and GPS132A techniques. The obtained results indicate that addition of nanomaterials to cement-based composites improves mechanical, electrical and nano-structural properties and the quality as well as emission factors of samples with optimization portion of nano-particles found by Response surface methodology (RSM) method.