Danse is by far the best companion, imo. The "mentor" idea is something you don't see often, his storyline goes to an interesting place and following that storyline gives you an opportunity to argue with the Brotherhood's hardcore ideals, which is something this game sorely lacks in many places. (Specifically the institute, whose bullshit you are never given the opportunity to properly challenge.)
Cait is also interesting, in that she undergoes a serious life change throughout the course of your interactions with her. Her personal growth makes her stand out a bit from the pack. Also, dat accent.
Nick is pretty cool. His struggles with his identity are kinda predictable, but it's cool that they were willing to give him some conflict on that point: one of the game's core questions is whether or not a synth's programmed personality is "real," and it's a good choice to have even a synth be unsure.
I like Piper's personality, but she has basically no story or personal progression, so it's hard to rank her high.
I'm not fan of the overall companion system, though. All video game relationships are reductive by their nature, but strengthening my bond with someone via picking locks near them seems like a new low.
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