Abstract: A new analytical procedure based on liquid scintillation counting(LSC) was developed for the determination of uranium in natural uranium samples. Factors possibly influencing the measurements of LSC were studied, such as α/β discrimination, quenching efficiency, and the optimum conditions for LSC were obtained, including pulse shape analysis （PSA） parameter and quenching correction curve. The results agree very well with the experimental results by volumetry. The precision and stability are fine with the s_r of 1.9% for 0.9857mg/g U(n=7). It is shown that LSC is an easy, efficient and accurate method capable of estimating uranium concentrations of various natural uranium samples in frontend of nuclear fuel cycle industry.