Developing practical strategies and a new reaction mode to access the versatile photocatalytic hydroalkylation of olefins with well-controlled regioselectivity remains highly desirable. Herein, we report a photoredox/nickel dual-catalyzed, regioselective hydroalkylation of unactivated alkenes by using toluene derivatives as alkyl sources, offering an efficient route for the selective construction of C(sp3)-C(sp3) bonds. This protocol features synthetic simplicity, avoidance of an external hydrogen source, and high regioselectivity, thereby expanding its potential utility in organic synthesis.