Well if you read any of my other postings you find that I have warm spot in my heart for the 216. Contrary to popular belief they can be hopped up but there are limits to revving because of the connecting rod lubrication.
But a critical part of the decision to invest into rebuilding/modifying a 'particular' engine is starting with something you know. I drove my 216 for 6 years before I pulled it and modified it. Rebuilding an inline six of any type is more expensive then a V8 build. Parts for SBC are ubiquitous and therefore cheap. Finding a machinist that will work on an antique can also be a challenge.
So my thought is why not just cleanup the 216 - put a coat of paint on it and put it back. It runs! Now your available funds can be focused on anything else that the car needs to be made road worthy and presentable.
Once complete now you can drive it around and enjoy it while you hunt for a reasonably priced 261 core.