The ATLAS detector at the Large Hadron Collider has been used to measure jet substructure modification and suppression in Pb+Pb collisions at a nucleon–nucleon center-of-mass energy √sNN = 5.02 TeV in comparison with proton–proton (pp) collisions at √s = 5.02 TeV. The Pb+Pb data, collected in 2018, have an integrated luminosity of 1.72 nb−1, while the ppdata, collected in 2017, have an integrated luminosity of 260 pb−1. Jets used in this analysis are clustered using the anti-kt algorithm with a radius parameter R = 0.4. The jet constituents, defined by both tracking and calorimeter information, are used to determine the angular scale rg of the first hard splitting inside the jet by reclustering them using the Cambridge–Aachen algorithm and employing the soft-drop grooming technique. The nuclear modification factor, RAA, used to characterize jet suppression in Pb+Pb collisions, is presented differentially in rg, jet transverse momentum, and in intervals of collision centrality. The RAA value is observed to depend significantly on jet rg. Jets produced with the largest measured rg are found to be twice as suppressed as those with the smallest rg in central Pb+Pb collisions. The RAA values do not exhibit a strong variation with jet pT in any of the rg intervals. The rg and pT dependence of jet RAA is qualitatively consistent with a picture of jet quenching arising from coherence and provides the most direct evidence in support of this approach.