In current work, a novel ultrasonic resonance plastic deformation (URPD) technique was firstly reported to effectively introduce high density of micro/nano deformation twins in a coarse-grained 316L stainless steel, which can simultaneously improve its strength and ductility (the uniform elongation increased from 49 ± 1.5% to 58 ± 2% and the ultimate strength increased from 600 ± 8 MPa to 670 ± 8 MPa). This approach is superior to many conventional strengthening methods for realizing a strength–ductility synergy in a metallic material while without obvious changing its geometry. The URPD technique is also thought applicable to other metallic materials.