This proof-of-concept study investigates the application of femtosecond laser-induced breakdown spectroscopy (fs-LIBS) for a rapid, almost non-destructive assessment of surface hardness of 80CrV2 steel samples subjected to thermal treatment. Conventional hardness testing methods, such as Vickers and Rockwell, often necessitate extensive sample preparation, geometric requirements and can alter the material's surface, limiting their effectiveness for rapid assessments. In contrast, LIBS offers a contactless approach that minimizes surface damage while providing high spatial resolution. In previous work, we have already shown that nanosecond laser-induced breakdown spectroscopy (ns-LIBS) leads to melt and material redeposition around craters, consequently reducing the achievable effective spatial resolution. To circumvent these problems, we used femtosecond laser pulses to generate reproducible plasmas on 80CrV2 steel samples with varying degrees of hardness. By maintaining consistent parameters such as laser energy, surface roughness, and planarity, this method facilitates the analysis of spectral changes associated with mechanical properties. Our results identify a correlation between the intensity ratios of iron emission lines and material hardness, underscoring the method's sensitivity to microstructural material changes. As expected, the femtosecond laser-induced breakdown spectroscopy technique (fs-LIBS) produced significantly smaller ablation craters than ns-LIBS. When accounting for the fluence changes resulting from crater formation and making the necessary adjustments, repeated measurements at the same locations could become feasible in the future. A method using fs-LIBS could be a compelling alternative for hardness testing of finely structured or heat-sensitive components.