The shift toward low-enrichment uranium (LEU) fuel for gas-cooled high-temperature reactors (HTRs) has revealed a lack of experimental data for validating neutronics codes that are used for the design and licensing of such systems. In the framework of the LEU-HTR experimental program at the PROTEUS critical facility, the safety-related effects of accidental moderation increase (ingress of water or other hydrogeneous compounds) in pebble-bed HTR core configurations employing low-enriched (16.7%) fuel were investigated. An important neutron balance component in this context is the integral reaction rate ratio of 238U capture (C8) relative to 235U fission (F5). It was necessary to develop new experimental techniques for the accurate measurement of C8/F 5 in the doubly heterogeneous fuel pebbles. These have involved the utilization of specially prepared particle foils on the one hand and the counting of whole fuel pebbles on the other. Core-center measurements employing both experimental methods have been carried out in two different HTR-PROTEUS configurations (with and without accidental moderation increase simulation, respectively). In each case, satisfactory agreement was obtained between the experimental results based on the two techniques. By carrying out a comparison of particle-foil C8/F5 measurements in the PROTEUS reactor's thermal column with the results of standard foil-activation measurement techniques, the systematic uncertainty (1) of the core-center measurements could be reduced by 0.6%, yielding a net experimental error of 1% with either of the new methods. A comparison of the experimental results with calculations based on the MICROX-2/ TWODANT codes in conjunction with JEF-1 cross sections has indicated that this calculational route overpredicts the-core-center C8/F5 value by 2.5% in both the investigated configurations.