KeithLaycockI have this mostly working now with some information not in the original post. Since my DFS Namespace server is on-prem, I needed to add a private endpoint to the Azure Files share, allowing on-prem to resolve to a private ip for the Azure file share over the S2S VPN. In addition, the AFS was also domain-joined as was described above.
I do have a DC in Azure now which makes this a bit easier, but once I understood how to properly configure DNS to conditionally forward requests on-prem to core.windows.net, things worked as I was hoping. This video was also helpful for that configuration. https://youtu.be/H04e9AgbcSc
Directions I used for private endpoint https://docs.microsoft.com/en-us/azure/storage/files/storage-files-networking-endpoints?tabs=azure-portal
Directions I used for AD join https://docs.microsoft.com/en-us/azure/storage/files/storage-files-identity-auth-active-directory-enable
So in the end I have an additional folder in the original DFS namespace which targets the Azure Files share and authenticates with AD. Looks pretty seamless.