Neural networks have been widely used as compensational models for aircraft control designs and as surrogate models for other optimizations. In the case of tiltrotor aircraft, the total number of aircraft states and controls is much greater than that of both traditional fixed-wings and helicopters. This requires, in general, a huge amount of training data for the network to reach a satisfactory approximation precision and makes the network size rise considerably. To solve the practical problem of reducing the size of the approximating network, efforts have to be made in the efficient utilization of the limited amount of training data. This work presents the methodology of optimizing the sample pattern of the training data set by adopting the metaheuristic algorithm of the particle swarm optimizer improved by the fourth-order Runge–Kutta algorithm. A 6-degree-of-freedom nonlinear flight dynamics model of the tiltrotor aircraft is derived, along with its approximation radial basis function neural network. An example case of approximating a highly nonlinear function is studied to illustrate the principle and main parameters of the optimizer, and the approximation performance of the time-domain response of the unstable nonlinear system is revealed by the study of a Van der Pol oscillator. Then, the presented method is applied to the modeled tiltrotor aircraft for its early and late conversion modes. The optimization scheme shows great improvement in both cases, as the function approximation error is reduced significantly.