In this thesis, the physical properties of certain multi-functional organic crystals were studied in detail. This study involves the growth of single crystals of Glucuronic acidγ-lactone (GAL), Imidazoliumtartarate (IMLT), (Bis)imidazoliumtartarate (BIMLT), and Diisopropylammonium iodide (DPI) and investigations of their optical, dielectric, piezoelectric, pyroelectric, and ferroelectric properties as a function of temperature and dependence on crystal structure in these organic crystals. Piezoelectric resonance was observed at certain frequencies when dielectric constant was monitored along the b-plate of GAL crystals. The electro-mechanical coupling coefficient estimated at the resonance near 1 MHz frequency revealed an exceptionally large value in GAL similar to that in inorganic lead titanate. The dependence of the piezoelectric resonance frequency on temperature was studied in detail. These crystals showed excellent second- and third-order nonlinear optical properties as well as high laser damage threshold. The high values of χ(2) andχ(3), laser damage threshold, and low UV cut-off makes GAL crystals an interesting prospect for NLO and laser applications. Towards this goal, GAL crystals were studied in detail with regard to determination of directions of dielectric axes, optic axes, and collinear phase-matching. Single crystals of another promising NLO organic crystal, IMLT were also grown which showed interesting dielectric, piezoelectric, and NLO properties. The dielectric dispersion with temperature provided an insight to the polarization mechanisms. Like GAL, IMLT also exhibits piezoelectric resonance. The existence of only one easy axis of vibration in IMLT enabled the candidate to identify the first resonance peak as corresponding to the fundamental mode of oscillation in the sample. This also helped to determine many piezoelectric parameters. By angular phase matching, one direction of phase matching in IMLT was identified. The conversion efficiency of IMLT along this direction was determined which was high in comparison to that in a standard KDP crystal. At piezoelectric resonance frequencies, the electro-optic response due to photo-elastic contributions is enhanced. Single crystals of organic ferroelectric BIMLT were grown by mixing two moles of imidazole with one mole of l-tartaric acid. The controversy with regard to the phase transition temperature of BIMLT was clarified by the DSC and structural analysis in this work. Previously, studies on BIMLT were limited to polycrystalline samples and single crystals with inclusions primarily due to the difficulty in growing good quality single crystals from aqueous solution. However, by experimenting the growth process using different solvents, good quality single crystals were achieved without the trapping of mother solution. This remarkable find is a notable result in these crystals for ferroelectric applications. The mechanism of ferroelectricity in BIMLT is mainly attributed to the transfer of protons along N–H---O hydrogen bonds in the direction of b-axis. Interestingly, the values of spontaneous polarization and Curie-temperature in the organic ferroelectric material DPI were significantly high and comparable to several popular inorganic ferroelectrics. The polarization obtained in this material is the highest among reported organic ferroelectrics. In addition to the high Curie temperature and spontaneous polarization, there were unique phase transitions that were revealed in DPI. The mechanism of ferroelectricity is quite complex, mainly being displacive type on account of the change in orientation of dipoles with electric field. Some contribution to ferroelectricity comes from the order-disorder nature of Nitrogen atom.