The material state dominated by the crystalline medium-range order (MRO) has been achieved in the diamond system, named paracrystalline diamond, guiding a new direction to explore the missing link between amorphous and crystalline states1. Since in metallic glasses the incorporation of MRO covering a comparable length scale with the shear transformation zone can stimulate the homogeneous plastic flow2, 3, 4, 5, manipulating the population of crystalline MRO motifs reaching the paracrystalline state in alloy systems would be conducive to tune their deformation behavior on nano-scale for retarding dominant shear bands. However, it is still profoundly challenging to tune MRO motifs in a controllable manner for achieving the paracrystalline state in alloy systems. Here, based on the vast composition space and the complex atomic interactions in the multicomponent and/or high-entropy alloys (HEAs)6, 7, 8, we present an “atomic-level tailoring” strategy, analogous to cutting paper into pieces, cutting the severe-distorted crystalline Zr-Nb-Hf-Ta-Mo HEA into the high-density crystalline MRO motifs on atomic-level, to create the unprecedented paracrystalline HEA. The addition of uniformly distributed Pt atoms with the large and negative mixing enthalpy into the pristine HEA induces the local atomic reshuffling around Pt atoms for the well-targeted local amorphization qualified as the “atomic-level scissors”. Such enthalpy-guided strategy coupled with lattice-distortion effect in HEAs can provide the unique atomic-level tailoring ability for numerous opportunities abound in the purposeful regulation of structural characteristics and the significant improvement of mechanical properties.