Abstract: Methods for making nuclear fuel compacts exhibiting low heavy metal contamination and fewer defective coatings following compact fabrication from a mixture of hardenable binder, such as petroleum pitch, and nuclear fuel particles having multiple layer fission-product-retentive coatings, with the dense outermost layer of the fission-product-retentive coating being surrounded by a protective overcoating, e.g., pyrocarbon having a density between about 1 and 1.3 g/cm.sup.3. Such particles can be pre-compacted in molds under relatively high pressures and then combined with a fluid binder which is ultimately carbonized to produce carbonaceous nuclear fuel compacts having relatively high fuel loadings.