In this work, quad-frequency precise point positioning (PPP) time and frequency transfer methods using Galileo E1/E5a/E5b/E5 and BDS-3 B1I/B3I/B1C/B2a observations were proposed with corresponding mathematical models. In addition, the traditional dual-frequency (BDS-3 B1I/B3I and Galileo E1/E5a) ionospheric-free (IF) model was also described and tested for comparison. To assess the proposed method for time transfer, datasets selected from timing labs were utilized and tested. Moreover, the number of Galileo or BDS-3 satellites, pseudorange residuals, positioning accuracy and tropospheric delay at receiver end were all analyzed. The results showed that the proposed quad-frequency BDS-3 or Galileo PPP models could be used to time transfer, due to stability and accuracy identical to that of dual-frequency IF model. Furthermore, the quad-frequency models can provide potential for enhancing the reliability and redundancy compared to the dual-frequency time transfer method.