When it is anticipated that data to be collected from an experiment cannot be adequately described by a low-order polynomial, alternative modelling and new design methods are required. Local linear regression, where the response is approximated locally by a series of weighted linear regressions, is an effective nonparametric smoothing method that makes few assumptions about the functional form of the response. We present new methods for the optimal design of experiments for local linear regression, including a new criterion, called DSI-optimality, to find designs that enable precise prediction across a continuous interval. Designs are found numerically for weights defined through the Gaussian and uniform kernels. Theoretical results are presented for the uniform kernel and the special case of prediction at a single point. The sensitivity of the designs to the choice of bandwidth in the local linear regression is studied, and it is found that designs for the Gaussian kernel with large bandwidth have a small number of distinct design points. The methodology is motivated by, and demonstrated on, an experiment from Tribology