Hi, In order to do MTS designs you have to read PG269 and become familiar with the clock distribution of the RFSoC device. That document has a section on Multi Tile Sync.
MTS involves using the XRFDC library to enable MTS. PYNQ provides a Python wrapper around the XRFDC library, so you can use Python to set up MTS mode. I don’t know of any examples online that provide working Python code to do that. Invoking the mode is really not all that complicated, understanding how to do the hardware design and work with the clock restrictions of MTS is a little more complicated.
There are no complete tutorials here on this forum yet. But there is a post for the 2x2 that discusses some of the fundamentals but is not entirely complete and ignores using Python to set the mode:
If you have a good hardware design and you have bare metal C working, then look through the PYNQ xrfdc library for the methods that you are using now. If they don’t exist then you will have to wrap them yourself just as in the example that you posted above.
It’s been on my chore list to create a MTS tutorial hardware design that works on a PYNQ RFSoC board but I have not found the time to do it. Don’t hold your breath for me 
Kind regards