One‐dimensional (1D) atomically thin crystals have attracted considerable interests due to their unique properties and potential applications. For example, reducing graphene physical size down to nanoscale to nanoribbons opens up band gaps, which makes graphene useful in electronic devices. Here, a facile approach to produce single‐ and bi‐layered MoS2 nanobelts by PMMA assisted decoupling of MoO2@MoS2 core–shell nanorods is reported by the authors. Atomic force microscopy (AFM), Raman and photoluminescence (PL) results show that the decoupled monolayer staple‐like MoS2‐shells can fold into bilayer nanobelts during the PMMA removal process. Raman, high‐resolution transmission electron microscopy (HRTEM) and selected area electron diffraction (SAED) results reveal that the left MoO2 nanorods exhibit high crystal‐quality. These findings provide a method to produce 1D MoS2 nanobelts, which have potential applications in electronics and catalysis.