New composites of waterborne polyurethane (WPU) as a matrix were prepared by incorporating rigid supramolecular nanoplatelets (SNs) as filler, which were self-assembled by the selective inclusion of β-cyclodextrin (β-CD) onto poly(propylene oxide) (PPO) segment in the poly(ethylene oxide)- block-PPO-block-poly(ethylene oxide) (PEO-b-PPO-b-PEO). It is worth noting that, when the loading level of SN is lower than 3wt%, the SNs with moderate PEO length result in the simultaneous increase in strength, elongation and Young's modulus in contrast with neat WPU. If there is no stretching free PEO chain, both strength and elongation decrease in spite of an increase in Young's modulus. However, too long PEO chains result in the decrease of mechanical performances while the relatively higher loading-level of SNs also inhibits the enhancement of strength and elongation.