The aim of Thrust 4 is to develop ground-breaking new materials that will underpin the Logic & Analog, Memory, and Interconnect themes of the SUPREME center. This theme will employ a materials-by-design paradigm, whereby data-driven materials discovery will be used to inform experimental synthesis and characterization. We are focusing on four materials classes: (i) 2D channel materials, e.g., TMDs and their heterostructures; (ii) wide and ultra-wide gap p-type channel materials, such as GaN and oxides; (iii) new ferroelectrics and highly-nonlinear optical materials, e.g. AlScN; (iv) protonated oxides for electrochemical synapses. Data-driven approaches include high-throughput first-principles calculations, physics-informed computational materials design, machine learning approaches, and AI-powered autonomous robotic synthesis and characterization.