The reasonable design of man-made multifunctional metamaterials with advanced mechanical and physical properties that are not found in nature is both challenging and important. In this paper, novel chiral structures are designed by adding V- and Tri- chiral elements to the typical hexagonal honeycomb substrate, so as to realize the modulation of in plane mechanical properties. Finite element simulations show that the Poisson's ratio of the hexagonal V-chiral structure is negative when the strain is greater than 0.4, and that of the hexagonal Tri-chiral structure is always negative. Quasi-static compression tests show that the introduction of chiral properties results in a stronger load-bearing capacity, and the hexagonal Tri-chiral structure has a stronger energy absorption (EA) and specific energy absorption (SEA) capability. A parametric study is carried out by means of FEM, by adjusting the geometrical parameters of the proposed structures, the performance in terms of energy absorption and compressive stiffness can be improved. Subsequently, Bloch-Floquet theorem is employed for the dispersion relations of the chiral metamaterials and the results show that compared to conventional hexagonal honeycomb, chiral metamaterials are able to generate band gaps in a lower frequency range. Numerical simulation results show that the bandwidth of the proposed novel chiral metamaterials can be tuned through a reasonable selection of hexagonal edge length, wall thickness and radius. Experimental investigations are conducted to test the vibration transmission rate of Structure Ⅲ, and the results prove that the structure is capable of vibration suppression in the target frequency band range. Finally, by filling Structure Ⅲ with steel columns, the structure generates band gaps in the lower frequency range, hence the application of this chiral metamaterial is broadened.