In recent works on the determination of pseudotachylyte within the principal slip zone (PSZ) of the Chelungpu fault (Taiwan), we demonstrated that frictional melting occurred at shallow depths during the 1999 Mw 7.6 Chi-Chi earthquake. Thus, the characteristics of melts are of paramount importance to investigate processes controlling dynamic fault mechanics during seismic slips. We conducted rock friction experiments on siltstone recovered from the Taiwan Chelungpu fault Drilling Project (TCDP) at a slip rate of 1.3 m/s and a normal stress of 1 MPa. Here we not only target to characterize experimental pseudotachylyte and evaluate the associated frictional behavior, but also compare it with natural frictional melts of TCDP. Our results show that (1) initial shear stress drop was related to the generation of low viscosity melt patches, (2) the evolution of shear stress in the postmelting regime was congruent with frictional melt rheology, and (3) the slip strengthening presumably resulted from the extremely low content of water of the frictional melt. In particular, the state-of-art of in situ synchrotron analyses (X-ray diffraction and Transmission X-ray Microscope) determine the presence of ultrafine spherical quartz (USQ) grains (~ 10 nm to 50 nm) in the glassy matrices presumably produced at high temperature. Our observations confirm that the USQ grains formed in rock friction experiments do occur in natural faults. We surmise the USQ is the result of frictional melting on siltstone and represents the latest slip zones of the Chelungpu fault, and further infer that the viscous melts may terminate seismic slips at shallow crustal conditions.