To promote biomass-derived tar and coke upgrading, biomass pyrolysis intensification was utilized by the co-pyrolysis of biomass and caking coal with suitable particle size. The intensification led to a 15% increase in light tar fraction in tar, indicating a transformation from heavy tar to light components (phenols, aliphatic hydrocarbons). Moreover, the resulting coke achieved high strength (M-25 > 80%) that can meet the requirement for moving bed gasification. To further facilitate tar upgrading and alleviate secondary reactions of volatiles that result in more secondary-coke and less gas, calcium-based Ca@Cu catalysts were synthesized and then loaded along the predicted coke cracks to improve tar quality without compromising coke granularity and strength. The results indicated that the catalytic upgrading mitigated the formation of pyrolytic water and secondary-coke, and dramatically improved tar quality as the light tar fraction in tar increased by 15-30%. Specifically, the upgraded light tar contains more phenols, naphthalenes, and anthracenes but less acids, ketones, and furfurals. It was postulated that selective cleavage of oxygen-containing functional groups (mainly ether bonds) promoted tar reconstruction to release more light aromatics during the catalysis. The coke strength continued to increase by 3-6%, possibly due to mitigation of H2O formation as indicated by more oxygen-containing groups retained in the aromatics during the Ca@Cu catalysis. The current study provided a new strategy to simultaneously upgrade coke and tar during catalytic pyrolysis of biomass for efficient utilization of the biomass.