In this paper, the catalysts of zirconium oxychloride on molecular sieve were prepared by immersion, and which was employed to catalyze the condensation reaction of 4-cyanopyridine and ethanol amine for synthesizing the pharmaceutical intermediates of 2-(pyridin-4-yl)-4,5-dihydrooxazole under solvent-free conditions. The resultants were identified by gas chromatography - mass spectrometry and the contents were determined by gas chromatography. The results indicated that, These catalysts all exhibit high catalytic activity. The activity is mainly derived from ZrOCl₂·8H₂O. It is also affected by the specific surface area of the carrier and the number of acidic sites. ZZrOCl₂·8H₂O/H-MCM-41 has the highest activity. By single factor multi-levels experiments, the optimal technology for the synthesis of 2-(pyridin-4-yl)-4,5-dihydrooxazole was obtained. The optimal conditions were as follow: the molar rate of 4-cyanopyridine to ethanol amine was 1:2, 10% ZrOCl2·8H2O/H-MCM-41 was used as catalyst, catalyst dosage was 10% mass of reactants, reacted at 110 ℃ for 3 h. Under the optimum technology, the conversion of 3-cyanopyridine was up to 98.4%.