Ultrasonic phase transfer catalysis system was developed for synthesis of 1-phenyl-1-cyclopropanecarbonitrile and its derivatives. Take the eneacetonitrile as the research model, the reaction conditions such as ultrasonic frequency, solvent, dosage of solvent, dosage of KOH, reaction time were studied. Results showed that the optimum reaction condition was as follows: 40 kHz, with 20 mL toluene as solvent, KOH and benzeneacetonitrile mole ratio of 10:1, reaction time 4 h. With yield of 95.6%, the 99.3% conversion was achieved. With high conversion (≥92.3%) and selectivity (≥92.2%), a variety of derivatives were synthesized. The system was also applied to the transformation of heterocyclic nitrile. Using 2-thiopheneacetonitrile as substrate, the 1-(thiophen-2-yl)cyclopropanecarbonitrile was synthesized with 95.2% conversion and 97.8% selectivity.