The present work aims at the toughening of DGEBA epoxy-cyanate ester hybrid with caprolactam and its subsequent reinforcement with different weight percentages of (1, 3, 5, and 7 wt%) 3-glycidylpropoxytrimethoxysilane functionalized Al-MCM-41 (F-Al-MCM-41) to fabricate F-Al-MCM-41 reinforced caprolactam toughened DGEBA epoxy-cyanate ester polymer nanocomposites. 1 H NMR and 13 C NMR data confirmed the formation of epoxy cyanate ester. Fourier transform infrared spectroscopy (FTIR) and differential scanning calorimetry (DSC) results ascertained the curing behaviour of polymer composites. Data from thermal and dielectric studies reveal that 7 wt% F-Al-MCM-41 reinforced caprolactam toughened DGEBA epoxycyanate ester exhibits superior thermal stability and dielectric constant than that of a neat composite. The SEM-EDAX analysis investigated the surface morphology of polymer composites. Data obtained from DMA showed that 7 wt% polymer nanocomposite possesses the highest storage modulus among the samples. K E Y W O R D S cyanate ester, epoxy, functionalized Al-MCM-41, polymer composites | 1907 JAYASREE Et Al.