Herein, we report on two-dimensional (2D) suprawavelength crystalline ZnO microstructures induced by a single ultraviolet (UV) femtosecond laser beam (400 nm, 35 fs, 666 Hz) with significant absorption enhancement. The achieved absorption values of 90-99% and 75-80% in the UV and visible spectral regions, respectively, were approximately 1.16 and 12 times higher than those of the blank ZnO crystal. Furthermore, large-area 2D ZnO microstructures were fabricated to be used as photodetectors (PDs). The experimental results demonstrated that, compared with the blank ZnO, these 2D ZnO microstructures effectively enhanced the PD performance by nearly four times at 375 nm. More importantly, the ZnO microstructure exhibited great response value, ∼7.12 A/W at 532 nm as well as acceptable response at 660 and 808 nm, whereas the blank ZnO crystal showed almost no response. Raman analyses demonstrated that no change occurred after the femtosecond laser induced the microstructure on ZnO. Thus, the enhancement in photoelectric performance can be attributed to the strong absorption of the ZnO microstructure.