We envisioned to develop new histone acylation catalysts that can regioselectively acylate other Lys residues than H2BK120 by moving the position of the DSH moiety on the LANA ligand from the N-terminus (LANA-DSH 1, Figure ) to an alternative position. As it was previously identified that Arg7 (R7) or Ser13 (S13) on LANA was not essential for its nucleosome binding, we substituted one of these amino acids with Lys, which was further conjugated with DSH at the ɛamino group (2-3, Figure ). In this case, CER was defined by the distance between the α-carbon atom of the Lys and the acyl carbon atom of the acyl pyridinium intermediate at the DSH moiety (Figure ). The radius of CER was 3.4-16.7 Å, based on MD simulation (Figure ).