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In this contribution, we propose the couple 1-Cyclohexylethanol/Acetophenone as a new biobased and bifunctional LOHC. This material shows promises for hydrogen storage by DFT modelling, while commercial catalysts were identified to carry out both hydrogenation and dehydrogenation: Ru/Al 2 O 3 was found to catalyse the complete hydrogenation of the LOHC at 115 °C in 2 h with 98% selectivity and, for the first time, Pt/C carries out the dehydrogenation at 205 °C in 36 h with total conversion but with a limited Degree of Dehydrogenation of 72%. The system was cycled three times during which up to 50% of the total hydrogen capacity was exploited, stable after 3 cycles. Kinetics experiments and DFT modelling of the reactions intermediates show that a system pairing C–O and C–C bonds is prone to degradation, due to side-reactions initiated by the O-moiety and the reversible hydrogenation of the C O bond during the dehydrogenation step. [Display omitted] • 1-Cyclohexylethanol/Acetophenone was proposed as a new biobased bifunctional LOHC. • Full hydrogenation and dehydrogenation were achieved with heterogeneous catalysts. • Energies of activation of each function was measured during the dehydrogenation. • Up to 53% of the total hydrogen capacity was exploited during the cycling. • DFT modelling rationalized the dehydrogenation pathway and degradation products. [ABSTRACT FROM AUTHOR]