This letter presents a measurement of the nuclear modification factor of large-radius jets in sqrt[s_{NN}]=5.02 TeV Pb+Pb collisions by the ATLAS experiment. The measurement is performed using 1.72 nb^{-1} and 257 pb^{-1} of Pb+Pb and pp data, respectively. The large-radius jets are reconstructed with the anti-k_{t} algorithm using a radius parameter of R=1.0, by reclustering anti-k_{t} R=0.2 jets, and are measured over the transverse momentum (p_{T}) kinematic range of 158<p_{T}<1000 GeV and absolute pseudorapidity |y|<2.0. The large-radius jet constituents are further reclustered using the k_{t} algorithm in order to obtain the splitting parameters, sqrt[d_{12}] and ΔR_{12}, which characterize the transverse momentum scale and angular separation for the hardest splitting in the jet, respectively. The nuclear modification factor, R_{AA}, obtained by comparing the Pb+Pb jet yields to those in pp collisions, is measured as a function of jet transverse momentum (p_{T}) and sqrt[d_{12}] or ΔR_{12}. A significant difference in the quenching of large-radius jets having single subjet and those with more complex substructure is observed. Systematic comparison of jet suppression in terms of R_{AA} for different jet definitions is also provided. Presented results support the hypothesis that jets with hard internal splittings lose more energy through quenching and provide a new perspective for understanding the role of jet structure in jet suppression.