Wow, quite a mishmash of tech going on there. 4 year old N class router, USB printer, Wireless repeater and Moca too. I am surprised it works at all.
Does the Smart TV and Home Theatre PC connect wireless or wired?
Why not connect the Brother printer with the LAN port instead of the finicky USB? Even wireless may be better?
I don't think you need the level of equipment you list, any current AC1900 class router or above will give you a much better wireless experience.
What is your budget for this network upgrade?
For hardware changes;
I would be looking to move the Printer off of the USB port (even consider buying a new one at this time for better per page costs and print speeds), getting rid of the repeater and running a few cable runs to where it is now (consider the flat Ethernet cable that is available) and buying a few 5 or 8 Port 1GBe switches to connect to a new AC Class1900 or higher router (you might even consider the RT-AC3200 for it's stable and effortless network handling, wired and wireless, that many people comment on here in the forums).
For the other changes;
I would be looking to wire the main router to a central location (and at least 10' above the ground level) in the areas (in 3D) that need to be covered. Don't forget to run at least 6 cable runs to that location for future expandability (one for each WAN/LAN port and an extra run too) and to finish each run near or at where the ISP's modem or cable is brought into the building.
You'll have a choice how to connect wired devices to your network. I would suggest a 5 or 8 port 1GBe switch on each router port (you'll decide if it's best to place these near the router or near the ISP's modem or cable drop location, depending on how much equipment is allowed to show when the router is installed for best WiFi performance).
Next, you can optimally configure the grouping of devices within each port so that the normal traffic the devices generate stay within the switch. For example, if the Camera writes to the NAS unit, they could be grouped together, along with a low bandwidth device like the printer (wired) for instance. You might also want to put the Main PC and the Home Theatre PC on different switches so that they have equal access to the NAS and the internet too without one negatively affecting the other.
With the cabling completed, the AC class router optimally located and having as many stationary devices wired or set to connect to the 5GHz band as possible with the remaining devices connecting to the 2.4GHz band, you can now test for the best channels to use for your specific environment.
To do this simply use manual channel selection in the router for the band you're optimizing and test each channel as thoroughly as you want to (some customers test each channel over a period of a few days to a week and see if they notice any improvements or not). The 2.4GHz band channels you want to test is 1, 6 and 11. For the 5GHz band the testing is the same, but you don't have to skip channels as they are far enough apart to not overlap on each other.
Again, do you have a budget? Any skills or willingness to do some of the work yourself? I hope I answered your concerns at least partially. Come back with more questions as needed.