Air-coupled ultrasonic testing systems are usually restricted by low signal-to-noise ratios (SNR). The use of pulse compression techniques based on P4 Polyphase codes can improve the ultrasound SNR. This type of codes can generate higher Peak Side Lobe (PSL) ratio and lower noise of compressed signal. This paper proposes the use of P4 Polyphase sequences to code ultrasound with a NDT system based on air-coupled piezoelectric transducer. Furthermore, the principle of selecting parameters of P4 Polyphase sequence for obtaining optimal pulse compression effect is also studied. Successful results are presented in molded composite material. A hybrid signal processing method for improvement in SNR up to 12.11 dB and in time domain resolution about 35% are achieved when compared with conventional pulse compression technique.