Carbon-based nanomaterials (CBNs) are showing significant potential in various fields, such as electronics, energy, and mechanics. However, their practical applications face synthesis challenges stemming from the complexities of structural control, large-area uniformity, and high yield. Current research methodologies fall short in addressing the multi-variable, coupled interactions inherent to CBNs production. Machine learning methods excel at navigating such complexities. Their integration with automated synthesis platforms has demonstrated remarkable potential in accelerating chemical synthesis research, but remains underexplored in the nanomaterial domain. Here we introduce Carbon Copilot (CARCO), an artificial intelligence (AI)-driven platform that integrates transformer-based language models tailored for carbon materials, robotic chemical vapor deposition (CVD), and data-driven machine learning models, empowering accelerated research of CBNs synthesis. Employing CARCO, we demonstrate innovative catalyst discovery by predicting a superior Titanium-Platinum bimetallic catalyst for high-density horizontally aligned carbon nanotube (HACNT) array synthesis, validated through over 500 experiments. Furthermore, with the assistance of millions of virtual experiments, we achieved an unprecedented 56.25% precision in synthesizing HACNT arrays with predetermined densities in the real world. All were accomplished within just 43 days. This work not only advances the field of HACNT arrays but also exemplifies the integration of AI with human expertise to overcome the limitations of traditional experimental approaches, marking a paradigm shift in nanomaterials research and paving the way for broader applications.