Abstract: Measurements of jet substructure in Pb+Pb collisions provide key insights into the mechanism of jet quenching in the hot and dense QCD medium created in these collisions.This Letter presents a measurement of the suppression of large-radius jets with a radius parameter of R = 1.0 and its dependence on the jet substructure. The measurement uses 1.72 nb(-1) of Pb+Pb data and 255 pb(-1) of pp data, both at root s(NN) = 5.02 TeV, recorded with the ATLAS detector at the Large Hadron Collider. Large-radius jets are reconstructed by reclustering R = 0.2 calorimetric jets and are measured for transverse momentum above 200 GeV. Jet substructure is evaluated using charged-particle tracks, and the overall level of jet suppression is quantified using the jet nuclear modification factor (R-AA). The jet R-AA is measured as a function of jet p(T), the charged k(t) splitting scale (root d(12)), and the angular separation (Delta R-12) of two leading sub-jets. The jet R-AA gradually decreases with increasing root d(12), implying significantly stronger suppression of large-radius jets with larger k(t) splitting scale. The jet R-AA gradually decreases for Delta R-12 in the range 0.01-0.2 and then remains consistent with a constant for Delta R-12 greater than or similar to 0.2. The observed significant dependence of jet suppression on the jet substructure will provide new insights into its role in the quenching process.