Theoretical calculations for jet substructure observables with accuracy beyond leading-logarithm have recently become available. Such observables are significant not only for probing a new regime of QCD at a hadron collider, but also for improving the understanding of jet substructure properties that are used in many searches for physics beyond the Standard Model. In this talk, we discuss a first measurement of such jet substructure quantities. The soft drop mass is measured in dijet events with the ATLAS detector at 13 TeV, unfolded to particle-level and compared to Monte Carlo simulations. We also present a measurement of substructure variables in ttbar and inclusive jet events, using data collected by the ATLAS experiment at 13 TeV. The measurements are performed with large-radius jets. They are corrected for detector effects, represented as particle-level distributions and are compared to the predictions of various Monte Carlo event generators. If available, a measurement of jet substructure observables performed using charged particles, at 13 TeV, is also presented. New event generator configurations for the modelling of jet production, derived using ATLAS data will also be presented.