If you were originally an Excel/Word user who switched to Docs/Sheets, for reasons other than cost, you would probably be better off sticking with Google's product. This is particularly true if you use Google's products for collaboration.
LibreOffice is better for people who are looking for a powerful office suite and primarily deal with printed documents (or handle electronic documents much like printed ones). It is best compared to Microsoft Office: Writer is very similar to Word, though Writer is better thought out in my opinion; Calc is very similar to Excel, though Excel seems to have better options for data visualization.
- text boxes in Writer
- vector graphics support (pdf, svg, ...)
- LibreOffice Draw, which there really isn't any equivalent to anywhere (it focuses on both drawing and text, while most vector drawing apps generally suck at text while Draw doesn't)
- higher performance with very big spreadsheets ("this should have been a SQLite file")
- Self-installed fonts
However, I do typically just use Google Docs when I don't need any of those. The recently added autocomplete feature finally did it for me.