2D materials offer the opportunity for continued device scaling while avoiding the short-channel effects that hinder bulk semiconductors. Due to their high surface areas, chemical modification is a powerful strategy for tuning the electronic properties of 2D semiconductors, although their dangling-bond-free surfaces present challenges to stable, uniform covalent functionalization. Northwestern University MRSEC IRG-2 has overcome these challenges by electrophilically trifluoromethylating 2D semiconducting WSe2 and MoS2 using the reagent trifluoromethyl thianthrenium triflate.