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Purpose: This study aimed to evaluate the effect of samarium-153-EDTMP (153Sm-EDTMP) on pain relief bone metastases of Breast Cancer (BC) and Prostate Cancer (PC) patients. Materials and Methods: Thirty patients aged 40-77 years (62.6±10.2 years) with intractable metastatic bone pain were included in the current study. A checklist of patient information and a standard questionnaire for the assessment of pain and quality of life were completed before and after four and eight week’s palliative treatment with 37 MBq/kg of 153Sm-EDTMP. To analyse the data, parametric and non-parametric tests were used in SPSS software. Results: Twelve females with BC (40%) and 18 males with PC (60%) were included. Four and eight weeks after palliative treatment of 153Sm-EDTMP, the mean pain score reduction and quality of life were statistically increased compared to before the intervention (P-value < 0.05). Notably, the amount of pain reduction in the fourth week was more than in the eighth week; however, the quality of life was better in the eighth week, without significant variation (P-value <0.05). In addition, there was no statistically significant relationship between pain reduction and the type of primary diseases, BC, and PC (P-value >0.05). Conclusion: The injection of 153Sm-EDTMP had therapeutic efficacy for bone pain palliation in patients with diffuse bone metastases at the end of the 4th and 8th week post-infusion.