The aerodynamic characteristics of rectangular cylinders provide valuable references for many engineering structures. Aiming to investigate the characteristics of vortex-induced vibration (VIV) of this kind of bluff section cylinder, the three-dimensional (3D) large-eddy simulations (LES) were conducted on the flow around an elastically mounted rectangular cylinder with an aspect ratio of 4. A novel method for creating 3D meshes was introduced and validated by comparing the aerodynamic parameters and vibration amplitudes with those of experimental data. The mechanism of VIV was then investigated by examining the evolution properties (including the mean and fluctuating pressure, predominant frequency, and spanwise correlation) of distributed pressure at various amplitude-dependent VIV stages. Additionally, the contributing/inhibiting effect of wind load acting on specific regions around the cylinder’s surface on VIV was clarified by investigating the energy input or output. The results show that the vibration amplitude affects both static and fluctuating pressures, with a significant variation in these pressures observed during the amplitude-ascent stage. The distributed aerodynamic force is mainly due to self-excited forces resulting from the cylinder vibration during amplitude-ascent stage, whereas both self-excited forces and forcing forces are prominent during the amplitude-descent stage. Notably, the spanwise correlation coefficient displays its minimum value at the peak amplitude, even lower than that in the non-lock-in region, with the highest value occurring at the onset of the amplitude-ascent stage. The energy analysis revealed that the wind loads acting on the upstream of the cylinder's surface tend to enhance VIV, while those acting downstream tend to inhibit it.