We are entering a technological revolution in automated chemical synthesis and materials discovery. For many years, sequence-defined biomolecules such as peptides and oligonucleotides have been synthesized using automated techniques, but similar methods for synthetic molecules have lagged far behind. In our group, we use high-throughput, automated synthesis techniques to design and generate large libraries of sequence-defined, synthetic oligomers. We built a custom automated synthesis instrument based on Suzuki cross-coupling (protection-deprotection synthesis) to build molecules for a wide range of applications in organic electronic materials, fluorescent dyes, and mixed conductors. Precise control of chemical sequence in polymeric materials plays a direct role in bulk material properties such as charge transport and self-assembled structures. In this way, we are coupling automated synthesis with cutting-edge methods in AI-guided molecular design to discover new functional materials.