Six priests and bishops accompanied Tawadros on his six-day visit, aimed at congratulating the new Catholic Pope, Francis I.
The Coptic Church announced the pope's departure on Thursday.
Tawadros is also relatively new to his post, taking office last year. His predecessor made the last visit by a Coptic pope to the Vatican in 1973.
The Coptic and Catholic churches split in the fifth century over theocratic differences.
Christians comprise about 10 percent of Egypt's population. Copts complain that since the overthrow of longtime ruler Hosni Mubarak in 2011, discrimination and attacks against them have increased, especially with the rise of the Egypt's Muslim Brotherhood to power.
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