Molecular baskets 1⁶⁻–3⁶⁻, functionalized with α-amino acids at their rim, undergo photo-induced α-decarboxylations to give amphiphilic 4³⁻–6³⁻ assembling into nanoparticles. Nanoparticulate 4³⁻–6³⁻ possess greater affinities for complexing OPs (akin to sarin and cyclosarin) than monomeric 1⁶⁻–3⁶⁻. With the ability of nanoparticles to function in urine, our study sets the stage for creating novel nanocarriers capable of spatiotemporal sequestration of nerve agents or pesticides in competitive chemical environments.