Since the energy demand increases, the sources of fluid energy such as wind energy and marine energy have attracted widespread attention, especially vortex-induced vibrations excited by wind energy. It is well known that the lock-in effect in vortex-induced vibration can be applied to the piezoelectric energy harvester. Although numerous researches have been conducted on piezoelectric energy harvesting devices in recent years, a common problem of low bandwidth and harvesting efficiency still exists. In order to increase the response amplitude and decrease the threshold wind speed of vortex-induced vibration, a bionic attachment structure is proposed based on the experimental method. In the present work, twelve models are designed according to the size of pits and hemispheric protrusions which are added to the surface of a flexible smooth cylinder. Compared with the smooth cylinder which is taken as a carrier, the harvester with the bionic structure shows stronger energy capture performance on the whole. As the threshold speed decelerates from 1.8m/s to 1 m/s, the bandwidth, on the contrary, increases from 39.3% to 51.4%. Particularly, for the 10 mm pits structure with 5 columns, its peak voltage can reach 47 V, and its peak power can reach 1.21 mW with a resistance of 800 kΩ, 0.57 mW higher than that of the smooth cylinder. Comparatively speaking, the hemispherical projections structure figures with a much more different energy capturing characteristic. Starting from the column, the measured voltage of the hemispherical bionic harvester is much smaller than that of the smooth cylinder, with a peak voltage less than 15 V and a reducing bandwidth. However, compared with the smooth cylinder, hemispheric projections with 3 columns have a better energy capture effect with a measured voltage of 35V, a resistance of 800kΩ, and a wind speed of 3.097 m/s. Besides, its output power also enhances from 0.48 to 0.56 mW.