Some improvements of the detection sensitivity in pulse time interval analysis (TIA) based on selective extraction of successively - correlated decay events within millisecond order from random or background events, were established by the utilization of PSD, to reject /-pulses from -ones and a simple chemical procedure of radium separation, together with the use of well resolved scintillator. By applying the PSD, the contribution of -decay events was completely eliminated in both the -spectra and the TIA distribution curves as well as the improvement into clear energy resolution and the enhancement of detection sensitivity for the TIA. As a result, the TIA and -spectrometric analysis of226Ra-extract showed the existence of223Ra (Ac-series) and /-correlated events with correlated life (due to 0.16 ms due to214Bi()
214Po()) along with a singly well resolved -peak to be useful for the determination of226Ra (U-series). The difference of half-lives (145 and 1.78 ms) due to216Po and215Po (direct daughters of224Ra for Th-series and223Ra for Ac-series, respectively) was also proven for the possibility of the simultaneous determination of both correlated events by using the TIA/PSD combined with chemical separation and liquid scintillation counting method. Finally, the simultaneous determination of three natural decay series, which include U-, Th- and Ac-series nuclides, have been conveniently carried out for some environmental samples using the present method combined with225Ra yield tracer (Np-series).