The research of robotic autonomous radioactivity detection or radioactive source search plays an important role in the monitoring and disposal of nuclear safety and biological safety. In this paper, a method for autonomously searching for radioactive sources through mobile robots was proposed. In the method, by using a partially observable Markov decision process (POMDP), the search of autonomous unknown radioactive sources was realized according to a series of radiation information measured by mobile robot. First, the factors affecting the accuracy of radiation measurement during the robot’s movement were analyzed. Based on these factors, the behavior set of POMDP was designed. Secondly, the parameters of the radioactive source were estimated in the Bayesian framework. In addition, through the reward strategy, autonomous navigation of the robot to the position of the radiation source was achieved. The search algorithm was simulated and tested, and the TurtleBot robot platform was used to conduct a real search experiment on the radio source Cs-137 with an activity of 37 MBq indoors. The experimental results showed the effectiveness of the method. Additionally, from the experiments, it could been seen that the robot was affected by the linear velocity, angular velocity, positioning accuracy and the number of measurements in the process of autonomous search for the radioactive source. The proposed mobile robot autonomous search method can be applied to the search for lost radioactive sources, as well as for the leakage of substances (nuclear or chemical) in nuclear power plants and chemical plants.