The discovery of novel two-dimensional (2D) materials is a very attractive research direction that can have a profound impact on a variety of applications in energy, environmental science, catalysis, and electronics. The selective electrochemical extraction of atoms from layered 3D structures promises a significant expansion of the world of 2D materials beyond the widely explored layered structures with weak interlayer interactions. To advance a new process for the synthesis of 2D materials and accelerate their discovery, a multidisciplinary team of chemists, physicists, and materials scientists will combine state-of-the-art computational, experimental, and machine-learning techniques in a closed-loop paradigm inspired by the Materials Genome Initiative. The project also includes high school outreach programs and interdisciplinary training of the next-generation workforce to cover a broad spectrum from synthesis and characterization to theory and modeling of materials.