The influence of prior pack boriding on the microstructure and properties of nanobainitised X37CrMoV5-1 hot-work tool steel was investigated in the present work. Pack boriding was conducted at 950 °C for 4 h. Nanobainitising consisted of two-step isothermal quenching at 320 °C for 1 h, followed by annealing at 260 °C for 18 h. A combination of boriding with nanobainitising constituted a new hybrid treatment. The obtained material exhibited a hard borided layer (up to 1822 ± 226 HV0.05) and a strong (rupture strength 1233 ± 41 MPa) nanobainitic core. However, the presence of a borided layer decreased mechanical properties under tensile and impact load conditions (total elongation decreased by 95% and impact toughness by 92%). Compared with borided and conventionally quenched and tempered steel, the hybrid–treated material retained higher plasticity (total elongation higher by 80%) and higher impact toughness (higher by 21%). It was found that the boriding led to the redistribution of carbon and silicon atoms between the borided layer and substrate, which could influence bainitic transformation in the transition zone. Furthermore, the thermal cycle in the boriding process also influenced the phase transformations during subsequent nanobainitising.