Would say for me it's Volkov and Chitznoi. I remember playing those missions in RA1 and being super hyped to see how powerful they both were. Fast forward to MO and it really is a blast from the past, especially how they go and absolutely rip apart everything in their way on the ground. Not only do they pretty much have a complete and total reword but they also appear in a completely redone version of Recharger which is a very memorable missions for RA2. Pretty badass throughout the entire story and when you take it into multi-player or skirmish they are still a force to be reckoned with.
Second would probably be Libra. The idea of a psychic prodigy that could control and entire county on her own but is too moody and instead focuses of telekinetic powers and esentially a mental hate field is too much fun. The into mission for her was just to good. All that time waiting just to have her pretty much wreck everything. That is one hell of a first appearance.
Inversely my least favorite is probably Morales and Siegfried. Morales isn't bad game play wise, if a little bland since he is pretty much a cross between Jarmen Kell and Boris in function but those voice lines...It makes it really hard to play any mission where you need to control him for an extended period. Every line is screamed at the top of his lungs and comes off as hardcore cringe. On top of that it feels like with a bit more reservation you could still get the point across as a hotshot sniper with an attitude but as it stands now, way to cringey to even play.
The reason Siegfried shares the least favorite spot is first that he is very...bland. Really he kinda comes off as a standard chrono legionnaire who has different tech. I get that he was a scientist and he is supposed to play that off but even then it seems like he is kinda lacking in personality. Not to mention for in-game use he comes off as kinda useless much of the time. He moves super slow, his weapon is a slow-firing orb that has a travel time, he has trouble with anything fast moving and the biggest sin of all, he is a dirty, dirty, team killer. Seriously, i think duing missions and trying to use him in skirmish games i have lost more units to his own fire then he has actually managed to kill. It is not a problem i had with any of the other hero units but him.