Most machine learning algorithms require us to set up their parameter values before applying these algorithms to solve problems. Appropriate parameter settings will bring good performance while inappropriate parameter settings generally result in poor modelling. Hence, it is necessary to acquire the “best” parameter values for a particular algorithm before building the model. The “best” model not only reflects the “real” function and is well fitted to existing points, but also gives good performance when making predictions for new points with previously unseen values. A number of methods exist that have been proposed to optimize parameter values. The basic idea of all such methods is a trial-and-error process whereas the work presented in this thesis employs Gaussian process (GP) regression to optimize the parameter values of a given machine learning algorithm. In this thesis, we consider the optimization of only two-parameter learning algorithms. All the possible parameter values are specified in a 2-dimensional grid in this work. To avoid brute-force search, Gaussian Process Optimization (GPO) makes use of “expected improvement” to pick useful points rather than validating every point of the grid step by step. The point with the highest expected improvement is evaluated using cross-validation and the resulting data point is added to the training set for the Gaussian process model. This process is repeated until a stopping criterion is met. The final model is built using the learning algorithm based on the best parameter values identified in this process. In order to test the effectiveness of this optimization method on regression and classification problems, we use it to optimize parameters of some well-known machine learning algorithms, such as decision tree learning, support vector machines and boosting with trees. Through the analysis of experimental results obtained on datasets from the UCI repository, we find that the GPO algorithm yields competitive performance compared with a brute-force approach, while exhibiting a distinct advantage in terms of training time and number of cross-validation runs. Overall, the GPO method is a promising method for the optimization of parameter values in machine learning.