In dye-sensitized solar cells (DSSCs), the counter electrode (CE) plays a crucial role as an electron transfer agent and regenerator of the redox couple. Unlike conventional CEs that are generally made of glass-based substrates (e.g., FTO/glass), polymer substrates appear to be emerging candidates, owing to their intrinsic properties of lightweight, high durability, and low cost. Despite great promise, current manufacturing methods of CEs on polymeric substrates suffer from serious limitations, including low conductivity, scalability, process complexity, and the need for dedicated vacuum equipment. In the present study, we employ and evaluate a fully additive manufacturing route that can enable the fabrication of CEs for DSSCs in a high-throughput and eco-friendly manner with improved performance. The proposed approach sequentially comprises: (1) material extrusion 3-D printing of polymer substrate; (2) conductive surface metallization through cold spray particle deposition; and (3) over-coating of a thin-layer catalyzer with a graphite pencil. The fabricated electrodes are characterized in terms of microstructure, electrical conductivity, and photo-conversion efficiency. Owing to its promising electrical conductivity (8.5 × 104 S·m−1) and micro-rough surface structure (Ra ≈ 6.32 µm), the DSSCs with the additively manufactured CEs led to ≈2.5-times-higher photo-conversion efficiency than that of traditional CEs made of FTO/glass. The results of the study suggest that the proposed additive manufacturing approach can advance the field of DSSCs by addressing the limitations of conventional CE manufacturing platforms.