Co-pyrolysis of sludge and waste plastics is a long-term strategic approach for producing valuable fuels. However, sludge is characterized by a high protein content, which serves as a significant source of nitrogenous components in bio-oil. To improve the quality of pyrolysis products, the present study investigated the effect of low-density polyethylene (LDPE) on nitrogen transformation during the pyrolysis of sludge protein (SP). The study findings indicated that LDPE addition reduced the amount of solid residue owing to the interaction between SP and H radicals generated by LDPE pyrolysis. The thermal weight loss difference consistently remained below 0 when the SP-to-LDPE mixing ratio was 7:3, indicating that LDPE promotes the pyrolysis of SP. For the analysis of nitrogen-containing products during pyrolysis, LDPE addition significantly reduced the levels of nitrogen-containing compounds in the bio-oils of glutamate (Glu), histidine (His), and tyrosine (Tyr). Specifically, at 600°C, Glu, His, and Tyr in the bio-oils decreased by 31.4%, 33.3%, and 34.38%, respectively. No significant changes were observed in the nitrogen content within the pyrolysis char of Glu and His. However, all three amino acids exhibited a significant increase in the formation of NOx precursors due to the attack on the nitrogen positions of the heterocyclic nitrogen species by the H radicals generated by LDPE. This study contributes to research on the impact of LDPE on nitrogen migration and conversion during the pyrolysis of SP, laying the foundation for subsequent studies on pollutant removal reactions.