The efficient and non-derivatizing dissolution of natural biopolymers by ionic liquids (ILs) is poised to redefine the application of these ubiquitous and structurally robust materials on a grand industrial scale. In concert with this idea is Natural Fiber Welding (NFW), a technique which exploits the solvating properties of ionic liquids to partially dissociate the outer biopolymer layers in strands of fibrous thread, followed by solvent removal to collapse the structures in a reconfigured and entangled hydrogen bonding network. For cotton, this welding produces a layered motif of mesoporous cellulose atop a core of unmodified crystalline cellulose, creating a hierarchical structure which retains a semblance of the native biomaterial. Aggressive welding conditions increase the thickness and surface area of the mesoporous layer, though excessive welding leads to full dissolution of the crystalline core creating a tradeoff between an increase in surface area with loss of product integrity. In the present work, we seek to subvert aggressive welding conditions by supplementing dissolved cellulose as an additive in the welding solution. We will demonstrate how this extraneous cellulose can coat and weld to the underlying cotton substrate to increase the size of the amorphous shell around the crystalline core and, ultimately, bolster the mesoporous network and enhance the overall surface area. In addition, we will discuss how Raman-sensitive functionalization can be used to identify inclusion depth of the extraneous material and as a way to probe the potential for layer-by-layer deposition of functional cellulose during the NFW process.