The phenomenon of spray in crossflow is of relevance in gas turbine combustor development. The current work focuses on spray in crossflow rather than liquid jet in crossflow from the standpoint of enhancing fuel dispersion and mixing. Specifically, the first part of the work involves study of spray structure, droplet sizing, and velocimetry for sprays of water and ethanol in a crossflow under ambient conditions. Laser-based diagnostic techniques such as Particle/Droplet Image Analysis (PDIA) and Particle Tracking Velocimetry (PTV) are utilized. Using spray structure images, trajectory equations are derived by multi-variable regression. It is found that the spray trajectory depends only on the two-phase momentum ratio and is independent of other flow parameters. A generalized correlation for the spray trajectory is proposed incorporating the liquid surface tension, which is found to be effective for our data, with water and ethanol, as well as data on Jet-A from the literature for a wide variety of operating conditions. An interesting phenomenon of spatial bifurcation of the spray is observed at low Gas-to-Liquid ratios (GLRs). The reason for this phenomenon is attributed to the co-existence of large and highly deformed ligaments along with much smaller droplets at low GLR conditions. The smaller droplets lose their vertical momentum rapidly leading to lower penetration, whereas the larger ligaments/droplets penetrate much more due to their larger momentum leading to a spatial separation of the two streams. The second part of the study focuses on evaporating sprays in preheated crossflow. Experiments are conducted using ethanol, decane, Jet-A1 fuel, and a two-component surrogate for Jet-A1 fuel. The crossflow air is heated up to 418 K and the effect of evaporation is studied on spray trajectory and droplet sizes. Measured droplet sizes and velocities at two successive locations are used to estimate droplet evaporation lifetimes. Evaporation constant for the d2 law derived from the droplet lifetimes represents the first-ever data for the above-mentioned liquids under forced convective conditions. This data can be used to validate multi-component droplet evaporation models. The last part of the study focuses on Large Eddy Simulations (LES) of the spray in crossflow. The near-nozzle spray structure is investigated experimentally to obtain droplet size and velocity distributions that are used as inputs to the computational model. For the spray in crossflow under ambient conditions, trajectory and droplet sizes at different locations are compared with experimental results. While the predicted trajectory is found to be in good agreement with data, the predicted droplet sizes are larger than the measured values. This is attributed to the implicit assumption in the secondary breakup model that the droplets are spherical, whereas the experimental data in the near-nozzle region clearly shows presence of mostly ligaments and non-spherical droplets, especially for the low GLR cases. A modified breakup model is found to lead to improved agreement in droplet sizes between predictions and measurements. Overall, the experiments and computations have provided significant insight into spray in crossflow phenomenon, and have yielded useful results in terms of validated spray trajectory correlations, droplet evaporation lifetimes under forced convective conditions, and a methodology for simulation of airblast sprays.