Direct catalytic modifications of carbon-hydrogen (C-H) bonds, ubiquitous in organic molecules, represent a powerful strategy in organic synthesis. In the past decade, chemists have focused on the development of sustainable methods for functionalization of inert C-H bonds using cost-effective earthabundant 3d transition-metal catalysts. To fully harness the potential of this technology, however, it is essential to control the stereoselectivity of the C-H functionalization processes. This review describes developments in the emerging area of enantioselective functionalization of C-H bonds by 3d transitionmetal catalysts proceeding via inner-sphere C-H activation.