Yes, using molds to make truffles is a simple way to get a beautiful finish to your chocolate candy.
Your truffles will look a bit more elegant than simply dipping the truffles in chocolate or rolling the truffles in nuts, coconut, or cocoa powder, etc.
If you decide to use a square candy mold to make truffles, I hope you'll show us a picture of the finished chocolates! :)
My mom got me into this one! She made it (with my sisters and I) for Christmas a few years back. I will never forget that day! We had a blast in the kitchen.