Ionic self-assembled multilayers (ISAMs) can be formed by alternately dipping a substrate in anionic and cationic polyelectrolytes. Each immersion deposits a monolayer via electrostatic attraction, allowing for nanometer-scale control over film thickness. Additionally, ISAM films can be applied to arbitrary substrate geometries and can easily incorporate a variety of polymers and nanoscale organic or inorganic inclusions. The ISAM technique was used to tune and functionalize a rapid, sensitive fiber optic biosensor for textit{Brucella}, a family of bacteria that are detrimental to livestock and can also infect humans. The sensor was based on a turn-around point long period fiber grating (TAP-LPG). Unlike conventional LPGs, in which the attenuation peaks shift wavelength in response to environmental changes, TAP-LPGs have a highly sensitive single wavelength peak with variable attenuation. ISAMs were applied to a TAP-LPG to tune it to maximum sensitivity and to facilitate cross-linking of receptor molecules. Biotin and streptavidin were used to attach biotinylated hybridization probes specific to distinct species of textit{Brucella}. The sensor was then exposed to lysed cell cultures and tissue samples in order to evaluate its performance. The best results were obtained when using samples from textit{Brucella} infected mice, which produced a transmission change of 6.0 ± 1.4% for positive controls and 0.5 ± 2.0% for negative controls. While the sensor was able to distinguish between positive and negative samples, the relatively short dynamic range of the available fiber limited its performance. Attempts to fabricate new TAP-LPGs using a CO2 laser were unsuccessful due to poor laser stability. A second application of the ISAM technique was as a source of second-harmonic generation (SHG). SHG is a nonlinear optical process in which light is instantaneously converted to half its wavelength in the presence of intense electric fields. Localized surface plasmons (LSPs) in metal nanoparticles produce strong electric field enhancements, especially at sharp tips and edges, that can be used to increase SHG. Colloidally grown silver nanoprisms were deposited onto nonlinear ISAM films and conversion of 1064 nm Nd:YAG radiation to its 532 nm second-harmonic was observed. Little enhancement was observed when using nanoprisms with LSP resonance near 1064 nm due to their large size and low concentration. When using shorter wavelength nanoprisms, enhancements of up to 35 times were observed when they were applied by immersion, and up to 1380 times when concentrated nanoprisms were applied via dropcasting at high enough densities to broaden their extinction peak towards the excitation wavelength. A maximum enhancement of 2368 times was obtained when concentrated silver nanoprisms with LSP resonance around 900 nm were spincast with an additional layer of PCBS.