A call for a national mobilization—by academe, government and industry—to move the United States economy from mainly petroleum-based to more sustainably biologically-based, with 100+ billion gallons annually of transportation fuel and value-added chemicals and materials produced from biomass. Traditional plant-based agricultural and forestry commodities and new value-added markets can be simultaneously served without long-term negative impacts on each other, provided there is major biosource and bioprocess innovation for biobased industrial products. Benefits will be far-reaching, from self-sufficiency in transportation fuel, more sustainable industries, revitalization of rural economies and improved balance of payments, to mitigation of environmental problems. Targets for biosources, processes and costs are proposed as well as an integrated structure for success by 2025.