As the demand for high-frequency and high-power electronic devices has increased, gallium nitride (GaN), particularly in the context of high-electron mobility transistors (HEMTs), has attracted considerable attention. However, the ‘self-heating effect’ of GaN HEMTs represents a significant limitation regarding both performance and reliability. Diamond, renowned for its exceptional thermal conductivity, represents an optimal material for thermal management in HEMTs. This paper proposes a novel method for directly depositing diamond films onto N-polar GaN (NP-GaN) epitaxial layers. This eliminates the complexities of the traditional diamond growth process and the need for temporary substrate steps. Given the relative lag in the development of N-polar material growth technologies, which are marked by surface roughness issues, and the recognition that the thermal boundary resistance (TBRGaN/diamond) represents a critical factor constraining efficient heat transfer, our study has introduced a series of optimizations to enhance the quality of the diamond nucleation layer while ensuring that the integrity of the GaN buffer layer remains intact. Moreover, chemical mechanical polishing (CMP) technology was employed to effectively reduce the surface roughness of the NP-GaN base, thereby providing a more favorable foundation for diamond growth. The optimization trends observed in the thermal performance test results are encouraging. Integrating diamond films onto highly smooth NP-GaN epitaxial layers demonstrates a reduction in TBRGaN/diamond compared to that of diamond layers deposited onto NP-GaN with higher surface roughness that had undergone no prior process treatment.