Vortex-induced vibrations of two mechanically coupled circular cylinders with asymmetrical stiffness in side-by-side arrangements are numerically investigated in a uniform flow at a low Reynolds number of 100. The oscillation system is restricted to the cross-flow direction, giving rise to a coupled two-degree-of-freedom response. Attention is placed on the two cylinders with a center-to-center gap ratio of 4 and a mass ratio of 10. The flow dynamics are described by the two-dimensional incompressible Navier–Stokes equations and resolved by the Characteristic-Based-Split finite element method. The stiffness of the first spring that connects the lower cylinder to the wall is chosen such that the vortex-induced vibration of the associated single cylinder with the same stiffness undergoes a pre-synchronization (state A), synchronization (state B) and post-synchronization (state C), respectively. In each state, the stiffness of the second spring connecting the lower and upper cylinders is varied to cover both synchronization and de-synchronization regimes. Numerical results show that the mechanically coupled system locks on the first-mode natural frequency in state A, while on the second-mode natural frequency in states B and C. In such a lock-in regime, the amplitude ratios of the two oscillating and coupled cylinders collapse well onto the corresponding first or second free-vibration mode. The overall coupling mechanism is further explained in terms of the hydrodynamic coefficients, frequency characteristics, wake patterns and effective added mass, quantifying the associated fluid-structure interactions against those governing a single-degree-of-freedom, single-cylinder system.