Definitely Tyrion Lannister. In a crossover with 'The Simpsons', he could bring his sharp wit and political acumen to Springfield. He'd probably outwit Mr. Burns in no time. His complex personality and ability to adapt would make for a very engaging character in such a crossover fanfiction.
Daenerys Targaryen would be a fascinating choice. In a crossover with 'Avatar: The Last Airbender', she could learn bending techniques and use them to her advantage. Her dragon - riding skills and her quest for the throne could be intertwined with the Avatar's world, creating a really unique and exciting story.
Arya Stark would be a great choice. She's already a skilled fighter in the ways of the Faceless Men. Training with samurai could enhance her skills even further. Her journey of self - discovery could be influenced by samurai teachings about honor and discipline.
I think Bran Stark could be very interesting too. As the Three - Eyed Raven, he has vast knowledge and powers. In a future fanfic, he could use his powers to foresee and prevent new disasters or to guide the future of Westeros in a more positive direction. However, his new powers might also make him a target for those who fear his influence.
Jon Snow would be an interesting character to be an avatar. Given his complex backstory and his role in the fight against the White Walkers, as an avatar he could gain even more powerful abilities. Maybe he could have the power to control the elements, which would be a huge advantage in battles. He could use this to create blizzards against the White Walkers or to put out fires during the sack of King's Landing.
Black Widow. She's a master spy and assassin. In the world of Game of Thrones, she could easily blend in with the various spies and informants. She could play the game of thrones better than most of the characters there, using her charm and combat skills to manipulate the situation to her advantage. She might even be able to uncover some of the deepest secrets of the Seven Kingdoms.
Jon Snow would also be a great addition. His journey from being a bastard to a leader in Game of Thrones could be paralleled in the world of Frozen. He could learn from Elsa about controlling his powers (if we assume he has some new ice - related powers in this crossover) and in turn, teach the people of Arendelle about loyalty and sacrifice, which are values he has held dear in Westeros.
Arya Stark in a 'Naruto Game of Thrones crossover fanfiction' would be fascinating. If she were to learn some of Naruto's ninja skills, she would become an even deadlier assassin. And Naruto's influence might change her path a bit, making her less vengeful and more about bringing real change to Westeros.
Daenerys Targaryen would be fascinating. She has her own dragons, but Lightbringer could be the key to truly uniting the people of Westeros under her rule. It could symbolize her rightful claim to the Iron Throne and be a tool to overcome any remaining opposition.
Arya Stark would be really interesting. She has the skills of a trained assassin. In the Fallout world, she could use her stealth and combat abilities to navigate the dangerous wastelands and take on raiders or other threats. Her ability to change her face could also come in handy for undercover operations or infiltrating enemy camps.
Definitely Cortana and Tyrion Lannister. Cortana is highly intelligent and has access to a vast amount of knowledge. Tyrion is known for his wits. They could form an alliance where Cortana provides strategic advice based on her analysis, and Tyrion uses his political acumen to make things happen. Their conversations would be really fascinating as they come from such different worlds but are both very clever.
One interesting combination could be Cole from Infamous and Jon Snow. Cole has his powers and moral dilemmas, and Jon Snow is all about honor and leadership. Their meeting could lead to some great discussions about power and responsibility. Another would be Fetch from Infamous and Arya Stark. Fetch's edgy nature and Arya's vengeful streak could make for an exciting duo.