Detailed neuroanatomical comparisons between humans and chimpanzees could greatly benefit evolutionary neuroscience. However, ethical considerations regarding primate research disallow acquisitions of chimpanzee MRI data in vivo for multiple years. Hence, the availability of diffusion MRI (dMRI) and tractography data from chimpanzees is limited to a few previously acquired datasets. Here we optimize diffusion acquisitions for an interdisciplinary approach to great ape neuroimaging, using post-mortem dMRI data from naturally deceased wild and captive animals. The optimization of data quality from two acquisition strategies allowed to us acquire chimpanzee diffusion MRI data of unpreceded quality and reopen a gateway for evolutionary neuroscience.