Improving the quality of Origin-Destination (OD) demand estimates increases the effectiveness of design, evaluation and implementation of traffic planning and management systems. The associated bilevel Sensor Location Flow-Estimation problem considers two important research questions: (1) how to compute the best estimates of the flows of interest by using anticipated data from given candidate sensors location; and (2) how to decide on the optimum subset of links where sensors should be located. In this dissertation, a decision framework is developed to optimally locate and obtain high quality OD volume estimates in vehicular traffic networks. The framework includes a traffic assignment model to load the OD traffic volumes on routes in a known choice set, a sensor location model to decide on which subset of links to locate counting sensors to observe traffic volumes, and an estimation model to obtain best estimates of OD or route flow volumes. The dissertation first addresses the deterministic route flow estimation problem given apriori knowledge of route flows and their uncertainties. Two procedures are developed to locate "perfect" and "noisy" sensors respectively. Next, it addresses a stochastic route flow estimation problem. A hierarchical linear Bayesian model is developed, where the real route flows are assumed to be generated from a Multivariate Normal distribution with two parameters: "mean" and "variance-covariance matrix". The prior knowledge for the "mean" parameter is described by a probability distribution. When assuming the "variance-covariance matrix" parameter is known, a Bayesian A-optimal design is developed. When the "variance-covariance matrix" parameter is unknown, Markov Chain Monte Carlo approach is used to estimate the aposteriori quantities. In all the sensor location model the objective is the maximization of the reduction in the variances of the distribution of the estimates of the OD volume. Developed models are compared with other available models in the literature. The comparison showed that the models developed performed better than available models.