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Miniature optical sensors that specifically identify low concentrations of environmental and biological substances are in high demand. Currently, there is no optical sensor that provides identification of the aforementioned species without amplification techniques at naturally occurring concentrations. Recently, it has been demonstrated that triangular silver nanoparticles have remarkable optical properties and that their enhanced sensitivity to their nanoenvironment has been used to develop a new class of optical sensors using localized surface plasmon resonance spectroscopy. The examination of both model and nonmodel biological assays using localized surface plasmon resonance spectroscopy will be presented in this review. It will be demonstrated that the use of a localized surface plasmon resonance nanosensor rivals the sensitivity and selectivity of, and provides a low-cost alternative to, commercially available sensors.