Data/Yar is next for me. It was only for one episode, but the legacy it left for Data throughout the show's run was so large. Plus the intoxicated Yar asking if Data was fully-functional always makes me smile.
Picard/Vash
Sisko/Jennifer
Bashir/Ezri
Worf/Ezri
Kira/Shakaar
Odo/Female Shapeshifter
Ishka/Zek
Leeta/Bashir
Leeta/Rom
Winn/Dukat
Janeway/Mark
Chakotay/Seska
Seven/Chakotay
Trip/T’Pol
Phlox/Feezal
Kelvin Uhura/Spock
Kelvin Sulu/Ben
Burnham/Tyler
Burnham/Book
Lorca/Cornwell
Adira/Gray
Jurati/Rios
Seven/Raffi
Narissa/Narek
Soji/Narek
Shaxs/T'Ana
Carol Freeman/Admiral Husband
Picard/Vash
Sisko/Jennifer
Bashir/Ezri
Worf/Ezri
Kira/Shakaar
Odo/Female Shapeshifter
Ishka/Zek
Leeta/Bashir
Leeta/Rom
Winn/Dukat
Janeway/Mark
Chakotay/Seska
Seven/Chakotay
Trip/T’Pol
Phlox/Feezal
Kelvin Uhura/Spock
Kelvin Sulu/Ben
Burnham/Tyler
Burnham/Book
Lorca/Cornwell
Adira/Gray
Jurati/Rios
Seven/Raffi
Narissa/Narek
Soji/Narek
Shaxs/T'Ana
Carol Freeman/Admiral Husband