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Tailoring electron transfer dynamics across solid-liquid interfaces isfundamental to the interconversion of electrical and chemical energy. Stackingatomically thin layers with a very small azimuthal misorientation to producemoir\'e superlattices enables the controlled engineering of electronic bandstructures and the formation of extremely flat electronic bands. Here, wereport a strong twist angle dependence of heterogeneous charge transferkinetics at twisted bilayer graphene electrodes with the greatest enhancementobserved near the 'magic angle' (~1.1 degrees). This effect is driven by theangle-dependent tuning of moir\'e-derived flat bands that modulate electrontransfer processes with the solution-phase redox couple. Combined experimentaland computational analysis reveals that the variation in electrochemicalactivity with moir\'e angle is controlled by atomic reconstruction of themoir\'e superlattice at twist angles <2 degrees, and topological defect AAstacking regions produce a large anomalous local electrochemical enhancementthat cannot be accounted for by the elevated local density of states alone. Ourresults introduce moir\'e flat band materials as a distinctively tunableparadigm for mediating electrochemical transformations.

Tunable electrochemistry with moir\'e flat bands and topological defects at twisted bilayer graphene