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Unsaturated C4 hydrocarbons are abundant in various petrochemical streams. They can be considered as a potential feedstock for the steam-cracking process, where they must be co-processed with C6 and higher (C6+) hydrocarbons of primary naphtha fractions. Co-pyrolysis experiments aiming at the comparison of different C4 hydrocarbon performances were carried out in a laboratory micro-pyrolysis reactor under standardized conditions: 820 °C, 400 kPa, and 0.2 s residence time in the reaction zone. C4 hydrocarbons were co-pyrolyzed with different co-pyrolysis partners containing longer hydrocarbon chain to study the influence of the co-pyrolysis partner structure on the behavior of C4 hydrocarbons. The yields of the pyrolysis products and the conversion of C4 hydrocarbons were used as the performance factors. A regression model was developed and used as a valuable tool for quantifying the inhibition or acceleration effect of co-pyrolysis on the conversion of co-pyrolyzed hydrocarbons. It was found that the performance of different C4 hydrocarbons in co-pyrolysis is substantially different from the separate pyrolysis of the individual components.