Large amplitude oscillatory shear (LAOS) coupled with Fourier transform rheology (FTR) was used for the first time to characterize the large deformation behavior of selected bituminous binders at service temperature. Two polymer modified bitumens (PMB) containing recycled EVA and HDPE and two unmodified bitumens were tested with LAOS-FTR. The LAOS-FTR response of all binders was compared at same frequency (experimental approach) and at either same Deborah number or same phase shift angle δ (rheological approach). In all the approaches, LAOS-FTR results allowed to differentiate between all the nonlinear mechanical characteristics of the tested binders.  All binders show LAOS-FTR patterns reminiscent from colloidal dispersions and emulsions. EVA PMB showed the lowest nonlinear levels compared to HDPE PMB, which is more prone to microstructural changes induced by the range of shear strains tested in LAOS.