In summary, this work demonstrated the feasibility of synthesizing gram-scale strained biaryl linkages by combining C-H biarylation and subsequent atroposelective Larock macrocyclization. Furthermore, this modular approach enabled the first total synthesis of micitide 982 (1). Notably, the use of Ac-Gly-OH as a ligand in C-H biarylation proved to be highly effective in this reaction. Moreover, it became possible to introduce any biaryl group into Nphthaloyl-L-alanine (19) in a single step. This method has proven to be effective not only in various analog syntheses but also in the synthesis of fluoro-pseudosporamide (42) with a highly strained fluoro atrop-linkage, which possesses non-natural, fluorine-substituted characteristics. The combination of C-H biarylation and atroposelective Larock macrocyclization in this modular approach is expected to be further developed for the synthesis of natural products with diverse biological activities and strained biaryl linkages in RiPPs.