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The high-regioselective synthesis of bisadducts based on low-symmetry C₇₀ has been a challenging work due to the large amount of formed regioisomers, which require tedious separation procedures for isomeric purity and block their application in different fields. Herein, we successfully obtained a novel 1, 2, 3, 4-bis(triazolino)fullerene[C₇₀] <b>2</b> with high regioselectivity by the rigid tether-directed regioselective synthesis strategy and the corresponding molecular structure was unambiguously confirmed by single-crystal X-ray crystallography characterization. The crystal data clearly show that the addition occurs at the domain of corannulene moiety at the end of ellipse C₇₀ as well as the 1, 2, 3, 4-addition sites located at one hexagonal ring with a [6,6]-closed addition pattern. Furthermore, 2 was applied as an additive of perovskite layer to construct MAPbI3-based regular (n-i-p) perovskite solar cells, affording the power conversion efficiency (PCE) of 18.59%, which is a 7% enhancement relative to that of control devices without additive.