Chiral metasurfaces can exhibit a strong circular dichroism, but it is limited by the complicated fabrication procedure and alignment errors. Here, a new type of selfâaligned suspended chiral bilayer metasurface with only oneâstep electron beam lithography exposure is demonstrated. A significant optical chirality of 221° ”mâ1 can be realized using suspended metasurfaces with a thickness of 100 nm. Furthermore, this study experimentally demonstrates that such a structure is capable of labelâfree discrimination of the chiral molecules at zeptomole level, exhibiting a much higher sensitivity (orders of magnitude) compared to the conventional circular dichroism spectroscopy. The fundamental principles for chiral sensing using moleculesâmetasurfaces interactions are explored. Benefiting from the giant chiroptical response, the proposed metadevice may offer promising applications for ultrathin circular polarizers, chiral molecular detectors, and asymmetry information processing.