* προπάππους (propappos): This is probably the closest single word, literally meaning "great-grandfather." It's commonly used.
* παππούς του παππού (pappous tou pappou): This translates to "grandfather of the grandfather," which is more explicit.
The best choice depends on the context. `προπάππους` is generally sufficient, but if you need absolute clarity, the longer phrase might be better.