There are only a few examples being reported for the simultaneous control of central chirality and axial chirality because it is more challenging. Herein, we report an iridium-catalyzed asymmetric hydroarylation of unactivated alkenes with heterobiaryls to simultaneously construct axial and central chirality. The reaction showed a broad substrate scope and delivered the products with satisfactory results. The results of the control experiments demonstrated that the FerroLANE ligand promotes the reaction to proceed along a specific modified Chalk-Harrod mechanism.