Nanosphere lithography (NSL) is an inexpensive, simple to implement, inherently parallel, high throughput, materials general nanofabrication technique capable of producing an unexpectedly large variety of nanoparticle structures and well-ordered 2D nanoparticle arrays. This article describes our recent efforts to broaden the scope of NSL to include strategies for the fabrication of several new nanoparticle structural motifs and their characterization by atomic force microscopy. NSL has also been demonstrated to be well-suited to the synthesis of size-tunable noble metal nanoparticles in the 201000 nm range. This characteristic of NSL has been especially valuable for investigating the fascinating richness of behavior manifested in size-dependent nanoparticle optics. The use of localized surface plasmon resonance (LSPR) spectroscopy to probe the size-tunable optical properties of Ag nanoparticles and their sensitivity to the local, external dielectric environment (viz., the nanoenvironment) is discussed