The process-property-microstructure relationship is investigated in the in-house fabricated unidirectionally reinforced PAN-phenolic C/C composites comprising surface-treated and untreated carbon fibers. The composites are subjected to a final heat treatment of 1000° or 2000°C. The mechanical properties of the composites are found sensitive to the process parameters (particularly the final HTT), as well as fiber surface condition (surface-treated or untreated). For the composites comprising surface-treated fibers, the flexural strength of the composites heat treated at 2000C is higher than that of the composites treated at 1000°C. For the composites with untreated fibers, the results are the opposite. Microstructure, particularly fiber-matrix morphology, has been used to explain the strength variation among the various C/C samples, as discussed in the text.