Despite the overwhelming critical and commercial success of the Marvel Cinematic Universe there has always been a constant criticism among most of the films; the villains are kind of weak.
This is no real surprise, considering most of the Marvel comics that the films were based on focused on the main hero and their personal struggles in life while the villains were simply meant as an obstacle for that hero to overcome. However, I still think that the MCU has had some pretty good villains throughout the years and I just wanted to list a few of them.
Just a heads up, I will not include Thanos on this list. While his presence has haunted the overarching narrative of the MCU, he hasn't done enough yet to be considered for this list.
5. Ultron ("Avengers: Age of Ultron")
This one is a bit of a controversial pick. While many fans felt that he didn't accurately embody the cold and unstoppable computer program from the comics, I wasn't really bothered by this since I'm not exactly a big fan of the comic version of Ultron. He's scary due to how unstoppable he feels and how cold his mechanical logic is, but to me he just wasn't that interesting and came across as a carbon copy of the Terminators from "The Terminator". However, the version found in "Avengers: Age of Ultron" is very fascinating to me. In the film, Ultron constantly struggles with his newly obtained sentience and the very human emotions (such as anger and betrayal). These emotions are portrayed phenomenally through Ultron's voice actor and motion capture actor James Spader. He managed to be a threat to the Avengers while still being interesting to watch.
4. The Winter Soldier ("Captain America: The Winter Soldier", "Captain America: Civil War")
I was very reluctant to put Winter Soldier on this list because I find it hard to classify him as a villain. Bucky Barnes (Sebastian Stan) is Steve Rogers' (Chris Evans) friend from World War II who was believed to be dead but reappeared in "Captain America: The Winter Soldier" as Winter Soldier; a soldier with a cybernetic arm who is brainwashed into working for the evil organization Hydra. We witness Bucky struggle with his actions as Winter Soldier and the mental conditioning Hydra put him through. He isn't evil because the actions he committed as Winter Soldier were against his will, yet he still committed those actions regardless. This is what makes him interesting as a character and antagonist, and I could bring myself to keep him off of this list, despite the fact that his villainy is questionable.
3. Red Skull ("Captain America: The First Avenger")
"Captain America: The First Avenger" is one the most underrated films in the MCU. The film does a fantastic job exploring the character Steve Rogers and his transformation into the hero Captain America. The same compliment extends to the villain. Red Skull (Hugo Weaving) is Captain America's arch nemesis. He represents everything Captain America stands against, so it makes sense that he's a Nazi (he's the leader of Hydra in the MCU, but they're basically Nazis). Red Skull also holds resentment toward Captain America for receiving a better version of the super soldier serum than he did (that's what made his face look like that). The power and accomplishments he has acquired leads him to believe he deserves that power more that a scrawny, goodhearted kid from Brooklyn. Like any fascist, he feels he deserves power and the fact that he has power is enough to justify him using it however he wishes. He can also be quite funny and entertaining to watch.
2. The Vulture ("Spider-Man: Homecoming")
"Spider-Man: Homecoming" was surprising for many reasons. One of which was that it had one of the best MCU villains in the form of Vulture (Michael Keaton). Vulture is interesting due to a certain level of sympathy you have for him. He was a construction worker who was tasked with cleaning up the destruction after "The Avengers". However, he and his workers are rendered unemployed after Tony Stark (Robert Downey Jr.) and his company take on the responsibility of cleaning up New York. Adrian Toomes/The Vulture take some of alien technology left over and make weapons out of them to sell on the black market. He does all of this to support his family and make sure they are living the good life. He isn't completely heartless, we see that he genuinely cares for his daughter, but we also see that he is willing to do anything for his family, up to and including murder. Like most great Spider-Man villains, he serves as a dark reflection of Peter Parker (Tom Holland). Both come from lower/working class backgrounds and both become alienated by the larger world around them (mostly by Stark). However, Peter decides to act selflessly, while Adrian acts (not selfishly) in favor of those close to him at the expense of anyone else.
1. Loki ("Thor", "The Avengers", "Thor: The Dark World", "Thor: Ragnarok")
You all knew he would be number one. Loki (Tom Hiddleston) is one of the most memorable and iconic villains to have spawned from the MCU. He was already known as the brother and nemesis of Thor (Chris Hemsworth) in the comics, but due to his appearances in the "Thor" films and "The Avengers" the character was transformed into a famous superstar. This mostly has to do with the amazing performance given by Tom Hiddleston. He is both intelligent and scheming, while being cowardly and unlucky at the same time. He is confident and dangerous one moment, only to have that confidence stripped away when one of the heroes (mostly Hulk) makes a baffoon out of him. He is sympathetic and relatable, while being a vicious, power-hungry murderer at the same time. He embodies everything we find so attractive about evil and at the same time he behaves like many of us would (inflated egos and a god complex) if we gained that same power. He also shows us how we would look ridiculous acting like self-absorbed divas and how both embarrassing and scary it would be to not have the self confidence needed to wield such power properly.