Abstract Twisted bilayer (TB) MoS2has attracted great interest due to its application in twistronics. A modification of the conventional growth method is usually required to overcome the energy barrier between layers to grow twisted bilayer MoS2 with different angle. Hence direct one-step synthesis of MoS2 with a large area, clean surface, and a wide twisted angle range is still a challenge. In this work, we show the direct growth of high-quality twisted bilayer and trilayer of MoS2 by a countercurrent physical vapor deposition (PVD) method. We investigated the evolution of optical properties of twisted MoS2 at the range from 0◦ to 60◦. Raman and photoluminescence (PL) results show a strong relationship between interlayer coupling and the twisted angle of bilayer MoS2. Moreover, interlayer exciton was observed in twisted bilayer MoS2 for a large twisted angle range below 253 K. In comparison, no interlayer exciton related emission was observed for transferred bilayer MoS2, indicating that bottom-up growth of twisted MoS2 presents better interlayer quality. Our results demonstrate a simple approach to produce twisted angle MoS2with high quality for twist-angle based optical and electronic properties investigations.