Air-coupled ultrasonic inspection is a noncontact and convenient nondestructive testing method. However, its vertical reflection method using a single probe (i.e., pulse-echo mode) is known to be difficult to achieve, even though it is frequently used inspection mode in conventional contact or water immersion ultrasonic testing. This is because the reflectivity of ultrasonic waves at the boundary between air and the surface of inspection object is enormous, and faint signals received after transmitting into the object are difficult to detect. In this study, in order to achieve the air-coupled ultrasonic single-probe reflection method, transmitting chirp signals (waves with a linearly frequency modulation) with an appropriate window function and applying a pulse compression technique (a cross-correlation process between the received signal and a reference chirp signal) was examined, and its effectiveness was investigated through experiments for polystyrene specimens. Experimental results showed that the proposed method was effective in detecting faint reflection signals after propagating through the specimens, and that the difference in plate thickness could be detected by observing the change of the signal-receiving period of multiple reflection signals between the top and bottom surfaces of the specimens. These results demonstrate the feasibility of nondestructive testing using the air-coupled ultrasonic vertical reflection method and could show an important step toward its future practical applications.