Synergistic effect in network formation of nylon-6(PA6) nanocomposites containing one dimensional(1D) multi-walled carbon nanotubes(CNTs) and two dimensional(2D) layered double hydroxide(LDH) platelets on improving the mechanical properties has been studied. Mechanical tests show that, with incorporation of 1 wt% LDHs and 0.5 wt% CNTs, the tensile modulus, the yield strength as well as the hardness of the ternary composite are greatly improved by about 230%, 128% and 110% respectively, as compared with neat PA6. This is mainly attributed to the unique, strong interactions between the CNTs and the LDHs as well as the jammed network-like structure thus formed between the nanofillers, as confirmed by the morphological observations. As compared with the binary nanocomposites, a much enhanced solid-like behavior in the terminal region of the rheological curves can clearly be observed for the ternary system, which also indicates the formation of a percolating filler network.