The technology of elastomer blends is largely focused on the choice of the ingredients and vulcanization conditions to achieve optimized properties after curing. Rubber curatives may have different degrees of solubility in each elastomer, leading to different concentrations and vulcanization rates in each phase depending on their composition. To achieve the targeted vulcanization, the understanding of the effect of curative components in each phase of the blend is desirable. Atomic Force Microscopy (AFM) allows the mechanical properties of the material’s surface to be probed with high-spatial resolution, providing complementary information on the morphology at the nanoscale. The full comprehension of the structure-property relationships in multiphase materials demands the acquisition of complementary local chemical information. In recent years, AFM's capabilities were increased by the combination of the technique with infrared (IR) spectroscopy, allowing for the obtainment of IR spectra and images with nanoscale resolution. This is useful for the identification of phases, tracking of changes over time and quantification of the content of chemicals in materials applied in different domains. In this work, we applied two AFM approaches, the Amplitude Modulated – Frequency Modulated (AM-FM) and the AFM-IR technique, for the thorough characterization of the effect of vulcanization systems on the phase-specific viscoelastic properties and chemical structure of polyisoprene/polybutadiene (PI/BR) blends. The variations of viscoelastic properties revealed by quantitative nanomechanical mappings were associated with the cross-link density evolution in the samples as a function of compound composition. IR mapping provided similar morphology images as well as complementary information of the effects of the variation of the curative contents through the observation of changes of the trans/cis ratio at the nanoscale.