PURPOSE: We aimed to develop an innovative RF coil toolset for high resolution in vivo and ex vivo non-human primate neuroimaging applications at 10.5T MRI. The main goal was to improve our multimodal neural connectivity pipeline through the improved SNR, CNR, and spatial resolution that result from utilizing high-density RF coil arrays in combination with ultra-high field MRI. METHODS: Two RF coil arrays, both comprising 8 transmit and 40 receive channels, were designed and built for in vivo and ex vivo NHP imaging at 10.5 T. Experimental data was collected on multiple in vivo and ex vivo specimens, showing the utility UHF MRI for NHP neuroscience. RESULTS: Experimental results demonstrate uniform whole-brain coverage within both in vivo-which included the cerebellar, and spinal cord regions-and ex vivo specimens. High spatial resolutions (in vivo: 0.1×0.1×0.5 mm, ex vivo: 120 micron isotropic ) were achieved, revealing detailed anatomical structures throughout. High temporal stability allowed for EPI and dMRI applications. CONCLUSION: An RF coil toolset comprising two 8ch transmit/40ch receive arrays was successfully designed for both in vivo and ex vivo NHP brain applications at 10.5 T. Both high-density RF coil arrays coupled with the SNR and CNR benefits available at UHF supported unmatched anatomical, functional, and diffusion applications at some of the highest spatial resolutions to date. Additionally, the combined capability of both in vivo and ex vivo MRI with the same brain specimen allows for tighter control for experimental-paradigm multistage studies examining translation between in vivo and ex vivo methodologies.