featuring metallic surface states surrounding an insulating bulk. The associated unique electronic structure of the helical Dirac surface states results in many exotic physical properties, such as the topological magneto-electric effect, [6] Majorana fermions, [7] and the quantum anomalous Hall effect. [8] However, because of the low formation energy of intrinsic defects, [9] the resulting bulk conductivity often obscures or even suppresses the desired TI behavior. [10][11][12] The realization of these novel topological phases requires high-quality TI thin films with sufficiently low defect concentration, typically obtained by molecular beam epitaxy growth. [13] Chemical vapor deposition (CVD) and polyol methods, which offer facile and cost-effective synthetic routes promising for large-scale device applications, have also received interest with successful demonstrations of the ambipolar field effect, [14] Aharonov-Bohm, [15,16] and Shubnikov-de Hass [17] oscillations in (Bi x Sb 1−x ) 2 Te 3 nano plates, as well as in Bi 2 Se 3 and Be 2 Te 3 nanoribbons. Nevertheless, the quantum Hall effect as a hallmark of Dirac surface states [18] has not yet been realized in these TI nanostructures. One possible reason might be the appreciable bulk conduction associated with Topological insulators (TIs) are quantum materials with topologically protected surface states surrounding an insulating bulk. However, defectinduced bulk conduction often dominates transport properties in most TI materials, obscuring the Dirac surface states. In order to realize intrinsic topological insulating properties, it is thus of great significance to identify the spatial distribution of defects, understand their formation mechanism, and finally control or eliminate their influence. Here, the electronic heterogeneity in polyol-synthesized Bi 2 Se 3 and chemical vapor deposition-grown Sb 2 Te 3 nanocrystals is systematically investigated by multimodal atomicto-mesoscale resolution imaging. In particular, by combining the Drude response sensitivity of infrared scattering-type scanning near-field optical microscopy with the work-function specificity of mirror electron microscopy, characteristic mesoscopic patterns are identified, which are related to carrier concentration modulation originating from the formation of defects during the crystal growth process. This correlative imaging and modeling approach thus provides the desired guidance for optimization of growth parameters, crucial for preparing TI nanomaterials to display their intrinsic exotic Dirac properties.Topological Insulators