© 2020 Hydrogen Energy Publications LLC Four, hot-rolled, plain-carbon steels with varying carbon content were subjected to slow strain-rate tensile (SSRT) tests in a 95-MPa gaseous hydrogen environment at ambient temperature. The influence of pearlite volume fraction on the magnitude of hydrogen-induced degradation of the materials’ strength and ductility was thereby determined. Hydrogen was seen to significantly affect strain-to-failure and reduction-in-area in all four materials, wherein such a loss of tensile ductility was ascribed to the premature initiation and subsequent propagation of surface micro-cracks as revealed by the quantitative damage evolution analyses on the post-fractured specimens. The pearlite grains on sample surfaces manifestly served as the preferential origins of hydrogen-induced micro-cracks, resulting in more considerable embrittlement in materials possessing a higher percentage of pearlite, due to the rapid coalescence of discrete embryonic damage during tensile straining.