The removal of uranium-233 (233 U) from the auxiliary charcoal bed (ACB) of the Molten Salt Reactor Experiment (MSRE), performed from January through May 2001, created both unique radiological challenges and widely-applicable lessons learned. In addition to the criticality concerns and alpha contamination, 233U has an associated intense gamma photon from the cocontaminant uranium-232 (232U) decaying to thallium-208 (208Tl). Therefore, rigorous contamination controls and significant shielding were implemented. Extensive, timed mock-up training was also imperative to minimize individual and collective personnel exposures. Back-up shielding and containment techniques (that had been previously developed for defense in depth) were used successfully to control significant, changed conditions. Additional controls were placed on tests and on recovery designs to assure a higher level of safety throughout the removal operations. This paper delineates the manner in which each difficulty was solved, while relating the relevance of the results and the methodology to other projects with high dose-rate, highly-contaminated ionizing radiation hazards. Because of the distinctive features of and current interest in molten salt technology, a brief overview is provided. Also presented is the detailed, practical application of radiological controls integrated into, rather than added after, each evolution of the project--thus demonstrating the broad-based benefits of radiological engineering and ALARA reviews. The resolution of the serious contamination-control problems caused by unexpected uranium hexafluoride (UF6) gaseous diffusion is also explicated. Several tables and figures document the preparations, equipment and operations. A comparison of the pre-job dose calculations for the various functions of the uranium deposit removal (UDR) and the post-job dose-rate data are included in the conclusion.