The vortex-induced vibration and energy harvesting of two cylinders in side-by-side arrangement with different attack angles are numerically investigated using two-dimensional unsteady Reynolds-Averaged Navier–Stokes simulations. The Reynolds number ranges from 1000 to 10,000, and the attack angle of free flow is varied from 0° to 90°. Results indicate that the vortex-induced vibration responses with attack angle range of 0°≤ α ≤ 30° are stronger than other attack angle cases. The parallel vortex streets are clearly observed with synchronized vortex shedding. Relatively large attack angle leads to a phase difference between the wake patterns of the two cylinders. Hydrokinetic energy can be obviously harvested when Re > 4000. Compared with the larger attack angle case, the two side-by-side cylinders with smaller attack angle have better performance on energy conversion. The maximum energy conversion efficiency of 21.7% is achieved. The optimum region for energy conversion is 5000 ≤ Re ≤ 7000 and 0°≤ α ≤ 30°.