Considering the extraordinary performance of water microdroplets in driving different reaction pathways from its bulk counterpart in the previous works, we performed several control experiments to elucidate whether aqueous or organic microdroplets drives the chemoselective double C-N cleavage. We first compared the microdroplet reaction of the imidazoline derivative 1a in chromatographic and anhydrous acetonitrile with trifluoromethanesulfonic acid (with the similar catalytic performance to sulfuric acid, see Entry 2 in Table ) as the acidic catalyst to avoid trace water from concentrated sulfuric acid and acetonitrile, and the result demonstrated no observable yield variations. we next monitored the double C-N breakdown of the imidazoline derivative 1a in aqueous microdroplets upon the introduction of water into acetonitrile. The result (Table , Entries 13-14) demonstrated that the double C-N cleavage was moderately retarded when more water was introduced. Similarly, the introduction of water into the reaction solution did not switch the reaction pathways in bulk although the conversion of 1a to 3a and 4a was prolonged as well as low conversion ratios (Figure ). A further screening of organic solvents demonstrated that the chemoselective double C-N cleavage of 1a can be realized by organic microdroplets by using all tested organic solvents (see the solvent optimization in Table , Entries 1-6). It confirmed that the chemoselective double C-N bond decomposition to form the vicinal diamine product 2a was driven by organic microdroplets rather than aqueous microdroplets. In other words, our study proved the strong power of organic microdroplet chemistry in driving extraordinary reactions as similar as aqueous microdroplet chemistry for the first time.