The invention relates to the technical field of nuclear radiation protection, and provides a one-button calibration control system and one-button calibration control method for a nuclear radiation calibration laboratory. The system comprises an operation station, a controller, a data processing display unit, a radioactive source control device, and a trolley, wherein the radioactive source controldevice is configured to place one or more radioactive sources, control the sourcing, expose the radioactive sources to establish a standard field, and shield the radioactive sources to close the standard field; and the trolley is configured to place the instrument to be calibrated, and adjust the distance of the instrument to be calibrated from the radioactive sources. Due to the method, only conventional true values to be calibrated need to be selected according to the scaling range of the meter, and a "one-button calibration startup" button is pressed to wait for the calibration to be completed, thereby obtaining the data collection record and a final calibration factor of each conventional true value to be calibrated. The invention is simple in coefficients and high in reliability.