The bending and shear behavior of RC beams strengthened with Carbon Fiber-Reinforced Polymers (CFRP) is the primary objective of this paper, which is focused on the failure mechanisms and on the moment-curvature response prior-to, and post, strengthening with different amounts and layouts of the CFRP reinforcement. Seven reinforced concrete beams were tested in 4-point bending, one without any CFRP reinforcement (control beam, Specimen C1), four with the same amount of CFRP in flexure but with different layouts of the reinforcement for shear (Specimens B1–B4), and two with extra reinforcement in bending, with and without reinforcement in shear (Specimens B6 and B5, respectively). During each test, the load and the mid-span deflection were monitored, as well as the crack pattern. The experimental results indicate that: (a) increasing the CFRP reinforcement above certain levels does not necessarily increase the bearing capacity; (b) the structural performance can be optimized through an appropriate combination of CFRP flexural and shear reinforcement; and (c) bond properties at the concrete–CFRP interface play a vital role, as the failure is very often triggered by the debonding of the CFRP strips. The experimental values were also verified analytically and a close agreement between the analytical and experimental values was achieved.