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The defect formation in two-dimensional WS₂ is presented, where nano angle-resolved photoelectron spectroscopy (nARPES) combined with scanning tunneling microscopy and scanning tunneling spectroscopy (STM/STS) measure a band gap renormalization. Non-contact atomic force microscopy also verifies local structure to enable deconvolution of acquired topographic images by STM. The formation of Tomonaga–Luttinger Liquids in mirror twin boundary (MTB) defects is shown with both nARPES and STS. A method is also presented that shows growth of one-dimensional (1D) MTBs from point defects, which are induced into WS₂ with Ar⁺ bombardment cycles. This methodology also provides a path to functionalize chalcogen sites. We show that 1D MTBs can be substantially charged at a local level due to the electronic structure of the substrate.