Nanocarbon networks, such as nanotubes and graphene, possess exceptional electronic, thermal, and mechanical properties, making them ideal for high-performance multifunctional materials. However, van der Waals connected networks reduce these benefits. Our group is investigating a novel carbon nanostructure and its network engineering process using external energies such as pulsed electric current and laser-induced shockwaves to address this. These processes enable us to tailor carbon-carbon sp2 molecular junctions between assembled nanocarbon structures, resulting in continuous novel sp2 molecular networks (ex: graphenenic nanoribbon) with substantial mechanical, thermal, and electrical property improvements. We believe that these molecularly engineered nanocarbon networks could have broader applications, particularly in strong and highly conductive multifunctional film and fibers for lightweight and high-performance composites, electronics, and energy storage device electrodes.