Certain ionic liquids have been shown to dissolve cellulose, other biopolymers, and even raw biomass under relatively mild conditions. This particular ability of some ionic liquids, accompanied by a series of concurrent advantages, enables the development of improved processing strategies for the manufacturing of a plethora of biopolymer-based advanced materials. The more recent discoveries of dissolution of lignocellulosic materials (e.g., wood) in ionic liquids, with at least partial separation of the major constituent biopolymers, suggest further paths towards the achievement of a truly sustainable chemical and energy economy based on the concept of a biorefinery which provides chemicals, materials, and energy. Nonetheless, questions remain about the use of ionic liquids and the advisability of introducing any new process which utilizes bulk synthetic chemicals which have to be made, disposed of, and prevented from entering the environment. In this article, we discuss our own journey from the discovery of the dissolution of cellulose in ionic liquids to the cusp of an enabling technology for a true biorefinery and consider some of the key questions which remain.