The upgrading of waste plastic pyrolysis oil (WPPO) through hydrotreating (HDT) is crucial for transforming plastic waste into chemical feedstock. The catalytic role of HDT is of paramount importance for this conversion procedure. In this study, bimetallic catalysts based on Ni and Mo were prepared using the surfactant-assisted melt-infiltration (SAMI) method, completely omitting the use of liquid solutions. Thorough analysis via X-ray diffraction, transmission electron microscopy, and hydrogen temperature-programmed reduction confirmed that the addition of Span60 surfactant effectively prevented the aggregation of Ni and Mo components, reduced the size of metal particles, and improved the dispersion of active sites on the zeolite supports. Consequently, NiMo-based catalysts incorporating Span60, synthesized using the SAMI method, exhibited a superior catalytic performance in the removal of nitrogen, sulfur, and chloride impurities from WPPO during HDT compared to those without surfactant. Specifically, the catalyst prepared with Span60 exhibited 15% higher nitrogen conversion compared to the catalyst prepared without Span60.