This work addresses the preparation, characterisation and screening of different Ni-Co catalysts supported on carbon nanofibres (CNFs) for use in the upgrading of bio-oil in supercritical water. The aim is to improve the physicochemical properties of bio-oil so that it can be used as a fuel. The CNFs were firstly oxidised in HNO 3 and afterwards subjected to a thermal treatment to selectively modify their surface chemistry prior to the incorporation of the metal active phase (Ni-Co). The CNFs and the supported catalysts were thoroughly characterised by several techniques, which allowed a relationship to be established between the catalyst properties and the upgrading results.The use of Ni-Co/CNFs for bio-oil upgrading in supercritical water (SCW) significantly improved the properties of the original feedstock. In addition, the thermal treatment to which the fibres were subjected exerted a significant influence on their catalyticproperties. An increase in the severity of the thermal treatment led to a substantial reduction in the oxygen content of the CNFs, mainly due to the removal of the less 2 stable oxygen surface groups, which allowed their surface polarity to decrease. This decrease resulted in less formation of solid products. However, it also reduced the H/C and increased the O/C ratios of the upgraded liquid. Therefore, a compromise between the yield and the properties of the upgraded bio-oil was achieved with a Ni-Co supported on a CNF with a moderate amount of oxygen surface groups.