We propose a new experiment design method to accelerate the recent novel diffusion-relaxation correlation spectroscopic imaging (DR-CSI) experiment. DR-CSI acquires imaging data across a range of different b-value and echo time combinations. This enables new insights into tissue microstructure, but the contrast encoding can be slow. Our experiment design approach selects a small subset of the most informative observations to acquire using results from estimation theory. We demonstrate with ex vivo mouse spinal cord MR data that the new experiment design approach enables DR-CSI to be accelerated by a factor of more than 2 without a substantial loss in quality.