A metal-free direct α-selective arylation of BODIPYs has been developed based on base-mediated C-H functionalization with easily accessible diaryliodonium salts, which provides a straightforward facile access to a variety of α-arylBODIPY dyes. The α-regioselectivity was confirmed by X-ray analysis, and was studied by DFT calculation. The resultant dyes show strong absorption and emission over a broad range of spectra tunable via the simple variation of the diaryliodonium salts.