Described herein is a chiral magnesium bisphosphate-catalyzed asymmetric double C(sp(3))-H bond functionalization triggered by a sequential hydride shift/cyclization process. This reaction consists of stereoselective domino C(sp(3))-H bond functionalization: (1) a highly enantio- and diastereoselective C(sp(3))-H bond functionalization by chiral magnesium bisphosphate (first [1,5]-hydride shift), and (2) a highly diastereoselective C(sp(3))-H bond functionalization by an achiral catalyst (Yb(OTf)(3), second [1,5]-hydride shift).