Spine metastases are a common and painful complication of cancer. A novel concept of treatment combines the in situ vertebroplasty with radiotherapy employing radioactive bone cement into the human vertebrae. Thus, investigations concerning possible bioactive and radioactive cements become a relevant theme. In this work, we have synthesized calcium phosphate bioceramics incorporated with Ho and Sm nuclides using sol-gel technique. Characterizations were performed using X-ray diffractometry, infrared spectroscopy, scanning electron microscopy, instrumental neutron activation analysis, and gamma spectroscopy. Results showed bioceramics composed by multiphasic calcium phosphates along with holmium and samarium phosphates, with 8.9 and 13.7 % of Sm and Ho in weight, respectively. After neutron activation, the Ho-166 and Sm-153 beta-emitters were identified and quantified on the bioceramics with activities estimated at 32.5 and 14.5 MBq/mg of Sm-153 and Ho-166 bioceramic powder, respectively. These radioactive calcium phosphate bioceramics can compose suitable radioactive cements to radiovertebroplasty.