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MoS₂/TiO₂-based nanostructures have attracted extensive attention due to their high performance in many fields, including photocatalysis. In this contribution, MoS₂ nanostructures were prepared via an in situ bottom-up approach at the surface of shape-controlled TiO₂ nanoparticles (TiO₂ nanosheets and bipyramids). Furthermore, a multi-technique approach by combining electron microscopy and spectroscopic methods was employed. More in detail, the morphology/structure and vibrational/optical properties of MoS₂ slabs on TiO₂ anatase bipyramidal nanoparticles, mainly exposing {101} facets, and on TiO₂ anatase nanosheets exposing both {001} and {101} facets, still covered by MoS₂, were compared. It was shown that unlike other widely used methods, the bottom-up approach enabled the atomic-level growth of well-defined MoS₂ slabs on TiO₂ nanostructures, thus aiming to achieve the most effective chemical interactions. In this regard, two kinds of synergistic heterojunctions, namely, crystal face heterojunctions between anatase TiO₂ coexposed {101} and {001} facets and semiconductor heterojunctions between MoS₂ and anatase TiO₂ nanostructures, were considered to play a role in enhancing the photocatalytic activity, together with a proper ratio of (101), (001) coexposed surfaces.