In this article a facile and green procedure for the synthesis of novel calcium silicate hydrated-nylon 6/66 nanocomposites is proposed. Calcium silicate hydrate (CSH) was synthesized by a hydrolysis technique assisted by ultrasound and using sodium dodecyl sulphate (SDS) as surfactant. CSH-nylon 6/66 nanocomposites were obtained by a solution mixing method at CSH loadings of 2.5, 25, 50 and 75 weight percent (samples CA, CD, CB and CC, respectively). The synthesis of CSH was confirmed by DRX and ATR-FTIR techniques; the CSH sample presents as mesoporous with a diameter between 3.34 nm and 52.68 nm and an average size of 27.07 nm; the specific surface area of the CSH sample was 343.99 m² g⁻¹. The formation of the CSH-nylon 6/66 nanocomposites was confirmed by ATR-FTIR, SEM, XRD, TGA, DSC and XPS techniques. The crystallization and melting temperatures (T_m and T_c, respectively) of CSH-nylon 6/66 nanocomposites occur at a slightly lower temperatures than those of neat Ny 6/66. These results suggest a slight decrease of the crystallite size and crystallization rate of nylon 6/66. The fusion enthalpy (ΔH_f) decreases with increase in CSH content in nylon 6/66, which can be associated to a good dispersion. The XRD peaks of the nylon 6/66 at 19.99° and 23.77° were displaced at slightly higher values of 2θ with the incorporation of CSH in the polymer forming nanocomposite materials.