9 Figuras, 4 Tablas.-- Material suplementario disponible en línea en la página web del editor. Co-pyrolysis of grape seeds and polystyrene was conducted in a fixed-bed reactor, followed by an analysis of the organic phase for possible further application as a drop-in fuel. Significant positive synergistic effects were found with the addition of polystyrene (5–40 wt%) to the conventional pyrolysis of grape seeds. There was a considerable improvement in the organic phase yield, in particular, reaching values over 80 wt%, markedly higher than those obtained from conventional pyrolysis (61 wt%). Fuel properties of the bio-oil were also upgraded, with a decrease in oxygen content and an increase in the heating value. An organic bio-oil fraction with pH values ranging from 5.4 to 6.2 was obtained, reducing the issues associated with handling bio-oils obtained from common pyrolysis of lignocellulosic biomass, usually ranging pH between 2 and 3. Finally, an increment in the desired compounds, mainly aromatics, was also attained, while at the same time achieving a low content of undesired compounds, such as phenols. It was demonstrated that polystyrene can act as a H2-donor, favoring oligomerization, cyclation and hydrodeoxygenation reactions into aromatic compounds. The authors would like to thank MINECO and FEDER for their financial support (Project ENE2015-68320-R). O.S.P acknowledges the FPI fellowship (BES-2016-077750) funded by MINECO. The authors would also like to thank the Regional Government of Aragon (DGA) for the support provided under the research groups support programme. Peer reviewed