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Molly Aya & Sophia Milagros
Molly Victoria & Sophia Veronika
Molly Victoria & Sopia Nikoleta
Molly Noelia & Sophia Natalie
Molly Johanna & Sophia Dorothy
Molly Martha & Sophia Kyra
Molly Harriet & Sophia Martha
Molly Radka & Sophia Hilary
Molly Alaia & Sophia Radka
Molly Hana & Sophia Beatrice / Beata
Molly Timea & Sophia Nora
Molly Patricia & Sophia Isobel
Molly Linnéa & Sophia Lilian
Molly Linnéa & Sophia Lilian
Molly Linnéa & Sophia Yasmin
Molly Linnéa & Sophia Violet

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Molly and Sophia are ok as twin names, though Molly seems a little more casual and nickname-y to me (though I don't mind it as a given name), whereas Sophia seems more formal and sophisticated. What about Mary and Sophia? Maria/Marie and Sophia?

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Molly Victoria and Sophia Caroline.

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Grant and Aiden are also just ok together, but they kind of sound like they come from different generations. I'd pair Grant with Adam, Gregory, or Brian and Aiden with Declan, Samuel, or Owen. But they're not so bad together.

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Grant Benjamin and Aiden Patrick.

Cute, but they are getting very common. I'm not sure if that's a problem or not.

Molly Katherine & Sophia Karin
Molly Stella & Sophia Esther
Molly Aurelia & Sophia Zlata
Molly Daphne & Sophia Kayla
Molly Deborah & Sophia Erlea
Molly Danica & Sophia Zora
Molly Susan & Sophia Lilian
Molly Elisabet & Sophia Isabella
Molly Leah & Sophia Tabitha
Molly Kveta & Sophia Hana
Molly Hannah & Sophia Grace
Molly Hannah & Sophia Maite
Molly Zita & Sophia Lada
Molly Veronika & Sophia Stephanie
Molly Victoria & Sophia Nikita

I think Molly and Sophia are mismatched even though I know they would both be currently considered 'trendy and feminine.' I think Margaret nn Molly and Sophia would be better suited. Looking at your list I think Eleanor and Sophia would be great. Some middle names you might like:
Molly Caroline and Sophia Emily
Molly Afton and Sophia Larkin

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Grant and Aiden are handsome together
Grant Stephen and Aiden Lucas
Grant Nicholas and Aiden Gregory

I think there's some imbalance in the pairs. I think Molly is very nicknamey and childish-sounding; I have a hard time seeing it on adults, especially professionals. On the other hand, Sophia sounds distinguished and IMO works throughout life. From your favourites list, I think Eleanor or Georgia would make a better set with Sophia, and Lauren or Bailey would fit better with Molly.

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The set Grant and Aiden works pretty well, but Aiden is so much more popular than Grant.

I don't particularly like them, but they're alright.

Molly Freya and Sophia Judith
Grant Stephen and Aiden Michael.

I like Grant. Aiden is also nice, though it seems its popularity exploded (in the US) over the past few years.

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Sophia is lovely. Molly is NMS... maybe as a nickname for Mary, though.

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MNs...

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Molly Isobel, Molly Olivia
Sophia Adelaide, Sophia Justine

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Grant Alexander, Grant Rhys, Grant Lucian
Aiden Rhys, Aiden Vincent, Aidan Henry

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Best of luck!