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Sulfur-containing functional π-conjugated cores play key roles in materials science, mostly due to their unique electrochemical and photophysical properties. Among these, the excellent electron donor tetrathiafulvalene (TTF) has occupied a central position since the emergence of organic electronics. Peripheral C–H modification of this highly useful sulfur-containing motif has resulted in the efficient creation of new molecules that expand the applications of TTFs. This Short Review begins with the development of the palladium-catalyzed direct C–H arylation of TTF. Subsequently, it summarizes the applications of this efficient C–H transformation for the straightforward synthesis of useful TTF derivatives that are employed in a variety of research fields, demonstrating that the development of a new reaction can have a significant impact on chemical science.  1	Introduction  2	Development of the Palladium-Catalyzed Direct C–H Arylation of TTF  3	Synthesis of TTF-Based Tetrabenzoic Acid and Tetrapyridine for MOFs  4	Synthesis of TTF-Based Tetrabenzaldehyde and Tetraaniline for COFs  5	Tetraarylation of TTFAQ  6	Synthesis of Multistage-Redox TTF Derivatives  7	Miscellaneous Examples  8	Conclusions

Catalytic C–H Arylation of Tetrathiafulvalenes for the Synthesis of Functional Materials