Graphene nanoribbons (GNRs), when synthesized with atomic precision by bottom–up chemical approaches, possess tunable electronic structure, and high theoretical mobility, conductivity, and heat dissipation capabilities, which makes them an excellent candidate for channel material in post-silicon transistors. Despite their immense potential, achieving highly transparent contacts for efficient charge transport—which requires proper contact selection and a deep understanding of the complex one-dimensional GNR channel-three-dimensional metal contact interface—remains a challenge. In this study, we investigated the impact of different electron-beam deposited contact metals—the commonly used palladium (Pd) and softer metal indium (In)—on the structural properties and field-effect transistor performance of semiconducting nine-atom wide armchair GNRs. The performance and integrity of the GNR channel material were studied by means of a comprehensive Raman spectroscopy analysis, scanning tunneling microscopy (STM) imaging, optical absorption calculations, and transport measurements. We found that, compared to Pd, In contacts facilitate favorable Ohmic-like transport because of the reduction of interface defects, while the edge structure quality of GNR channel plays a more dominant role in determining the overall device performance. Our study provides a blueprint for improving device performance through contact engineering and material quality enhancements in emerging GNR-based technology.