Drawing inspiration from hierarchical structures, axisymmetric design layouts were introduced, and hybrid hierarchical chiral structures (HHCS) based on four- and six-chiral structures were proposed. The performance of HHCSs under in-plane compression is investigated using finite element methods and experiments. The effect of different loading conditions on the behavior of HHCSs is discussed. Under low-speed impact, HHCSs exhibit a negative Poisson’s ratio (NPR) effect, which diminishes as the velocity increases and the inertial effects gradually become dominant. The parameter study shows that increasing the connectivity between subunits and the thickness can enhance the energy absorption capacity of the structure while maintaining a good NPR effect. The conventional inclined deformation mode of the chiral structure is improved by the axisymmetric layout, which effectively improves the energy absorption.