11Improving the interlaminar fracture toughness of fibre-reinforced composites based on thermosetting 12 polymeric matrices is of significant interest to a broad range of applications. In the present work we report a 13 multi-scale approach to synergistically toughen composites by combining nano-and macro-scale 14 reinforcements inspired by natural composite materials. Carbon reinforcements with two different length 15 scales are used: nano-scale carbon nanofibres (~100 nm diameter) and macro-scale carbon z-pins (~280 µm 16 diameter) to reinforce continuous carbon-fibre composites in the through-thickness direction. The resultant 17 composite, featuring three-dimensional reinforcement architecture, possesses triple toughening mechanisms 18 at three different scales, thus yielding a synergistic effect. At the nano-scale, the carbon nanofibres alone 19 promote high mode I delamination resistance (~70% increase in interlaminar fracture energy) by multiple 20 intrinsic and extrinsic toughening processes around the crack tip. The macro-size carbon z-pins, together 21 with the crossover continuous fibres, promote a strong extrinsic toughening mechanism (~200% increase in 22 the interlaminar fracture energy) behind the crack tip and over a larger length-scale via both the z-pins and 23 crossover fibres bridging the crack faces. When used concurrently, the nanofillers and z-pins promote a 24 higher toughness under quasi-static loading (~400% increase in fracture energy) than when used separately 25 due to a multiplicative effect from the interplay between intrinsic and extrinsic toughening processes 26 operative ahead of, and behind, the crack tip. Under mode I interlaminar cyclic-fatigue loading, the multi-27 scale laminates show a strong improvement in resistance against fatigue delamination growth. Similar to the 28 synergistic increase in fracture energy, a greater increase in the delamination fatigue resistance occurs when 29 both are active together. However, the results indicate that the synergistic effect of the multi-scale 30 toughening is statistically significant under quasi-static loading but not under fatigue loading. A very small 31 reduction (~2%) in the tensile strength is observed for the multi-scale reinforced laminates. 32 33