Does it matter which one I ground, whether it is the CT Cabinet or the Main Panelboard?
Picture for clarity:
Image ground-ct-or-main-panel hosted in ImgBB
ibb.co
Thanks for your help
You should probably clarify what you mean by "ground".
To elaborate on what infinity said, the main panelboard is required to have the neutral bonded there. For the CT cabinet you can either Bond it directly with/to the neutral, or you can run an SSBJ to the neutral in the main panel.
If you are talking about dirt/grounding electrodes, that connection can be made anywhere from the service point to the main panel (service disconnect).